Systems and methods for lithium metal electrode preparation

Abstract

Provided herein are methods and systems for preparing electrodes for rechargeable energy devices in a continuous two-step process. In certain aspects, this disclosure provides a two-step process for selective electrochemical extraction of lithium from an aqueous source comprising lithium, followed by electrochemical plating of lithium metal for use as a Li-metal battery electrode.

Description

SYSTEMS AND METHODS FOR LITHIUM METAL ELECTRODE PREPARATIONCROSS-REFERENCE

[0001] This application claims the benefit of U.S. Provisional Application No. 63 / 601,417, filed November 21, 2023 and U.S. Provisional Application No. 63 / 682,534, filed August 13, 2024, each of which application is incorporated herein by reference.BACKGROUND

[0002] The preparation of lithium metal electrodes plays a crucial role in the production of various lithium-based products. However, the current methods for lithium electrode preparation are often expensive, resource-intensive, and present challenges in achieving high purity and low defect electrodes. There have been considerable efforts to develop more efficient approaches to make the process more cost-effective, environmentally friendly, and accessible for widespread use. There are, however, unmet needs to overcome the inherent limitations of conventional methods. The present disclosure addresses these needs and offers related advantages.SUMMARY

[0003] In some aspects, provided herein is a method comprising: (i) contacting an aqueous source comprising lithium with an intermediate electrode; (ii) extracting and transferring the lithium from the aqueous source to the intermediate electrode to form a lithium-rich intermediate electrode; and (iii) transferring the lithium from the lithium-rich intermediate electrode to a current collector substrate to form an electrode for a rechargeable energy device. In some embodiments, the aqueous source comprising lithium is brine. In some embodiments, the aqueous source comprising lithium further comprises Na+, K+, Mg2+, Ca2+, B(OH)4, Fe2+, Fe3+, Mn2+, MnO , MnO4, CT, SO42’, NH3, NH4+, NH40H, NO2, HN02, NOf, an alkali metal ions, an alkali earth metal ions, or any combination thereof. In some embodiments, the aqueous source comprising lithium comprises a geological resource. In some embodiments, the aqueous source comprising lithium is pretreated to remove Na+, K+, Mg2+, Ca2+, B(OH)4, Fe2+, Fe3+, Mn2+, MnO42, MnO4, CT, SO42’, NH3, NH4+, NH40H, NO2, HN02, NO3’, an alkali metal ions, an alkali earth metal ions, or any combination thereof.

[0004] In some embodiments, (ii) is performed by connecting a counter electrode to the intermediate electrode in a circuit, using the aqueous source comprising lithium as an electrolyte.In some embodiments, (iii) is performed by applying an electric potential across the lithium-rich intermediate electrode and the current collector substrate. In some embodiments, the intermediate electrode in (i) is substantially free of lithium or is in a de-lithiated state. In some embodiments, the intermediate electrode comprises about 30 atomic % (at%) less than a maximum amount of lithium that can be present.

[0005] In some embodiments, the intermediate electrode is obtained from recycled lithium-ion battery materials. In some embodiments, the intermediate electrode is obtained from black mass produced from shredding lithium-ion battery materials. In some embodiments, the intermediate electrode comprises iron phosphate, manganese oxide, or nickel manganese cobalt oxide.

[0006] In some embodiments, the intermediate electrode comprises a metal current collector or a carbon current collector. In some embodiments, the intermediate electrode comprises the metal current collector. In some embodiments, the metal current collector comprises copper (Cu), titanium (Ti), aluminum (Al), magnesium (Mg), zinc (Zn), tin (Sn), vanadium oxide (V2O5), or any metal that is capable of forming an alloy with lithium. In some embodiments, the intermediate electrode comprises the carbon current collector. In some embodiments, the carbon current collector comprises graphite. In some embodiments, the intermediate electrode comprises an electrically conductive slurry comprising an electrically conductive additive. In some embodiments, the electrically conductive additive comprises carbon.

[0007] In some embodiments, the intermediate electrode is non-reactive with non-lithium components in the aqueous source. In some embodiments, the intermediate electrode is reactive with non-lithium components in the aqueous source. In some embodiments, the intermediate electrode and a nonaqueous / polymer electrolyte are physically separated from a counter electrode and the aqueous source comprising lithium by a lithium ion-selective membrane. In some embodiments, the lithium ion-selective membrane permits lithium ions to selectively flow through to the intermediate electrode.

[0008] In some embodiments, the lithium-rich intermediate electrode comprises lithium iron phosphate (LiFePC , LFP), lithium nickel manganese cobalt oxide (LiNiMnCoCh, NMC), lithium manganate (Li2MnO4, LMO), LiCe, LixMgy, LixAly, LixSiy, or a combination thereof.

[0009] In some embodiments, transferring the lithium from the aqueous source to the intermediate electrode in (ii) comprises intercalating the lithium in the intermediate electrode to form the lithium-rich intermediate electrode. In some embodiments, the lithium-rich intermediate electrode comprises at least 30 at% more than a minimum amount of lithium that can be present. In some embodiments, transferring the lithium from the lithium-rich intermediate electrode to thecurrent collector substrate in (iii) comprises delithiating the lithium-rich intermediate electrode. In some embodiments, the intercalating and the delithiating are reversible.

[0010] In some embodiments, the current collector substrate comprises copper, copper alloy, aluminum, aluminum alloy, titanium, titanium alloy, nickel, nickel alloy, stainless steel, carbonaceous material, or any combination thereof. In some embodiments, the copper alloy comprises Cu-Ni, Cu-Ti, Cu-Zn, Cu-Al, Cu-Sn, or any combination thereof. In some embodiments, the current collector substrate comprises Cu-Ni, Cu-Ti, Cu-Zn, Cu-Al, Cu-Sn, Ni- CO, Al -Mg, Fe-Cr-Ni, or any combination thereof.

[0011] In some embodiments, the current collector substrate comprises carbon, carbon paper, carbon cloth or a metal or noble metal mesh or foil. In some embodiments, the current collector substrate comprises a foil, a mesh, a cloth, or a foam.

[0012] In some embodiments, an electrical connection to the intermediate electrode is made via copper, copper alloy, aluminum, aluminum alloy, titanium, titanium alloy, nickel, nickel alloy, stainless steel, carbonaceous material, or any combination thereof.

[0013] In some embodiments, the transferring of the lithium from the lithium-rich intermediate electrode to the current collector substrate comprises electrodeposition of the lithium as a layer of lithium metal on the current collector substrate.

[0014] In some embodiments, the electrode is a battery-ready electrode.

[0015] In some embodiments, (i) and (ii) are carried out in a first chamber and (iii) is carried out in a second chamber that is different from the first chamber. In some embodiments, the intermediate electrode is delithiated after (iii) and returned to the first chamber for repeating (i) and (ii). In some embodiments, the method further comprises, after (ii) and before (iii), rinsing and / or drying the intermediate electrode. In some embodiments, the method further comprises, after (iii), re-using the intermediate electrode in (i). In some embodiments, the method further comprises after (iii), treating the electrode by refining or post processes. In some embodiments, the refining or post processes comprise cleaning, heating, or applying pressure on the electrode. In some embodiments, the refining or post processes comprise applying heat to the electrode at a temperature below about 150°C. In some embodiments, the refining or post processes comprise applying pressure on the electrode at most 5 MPa.

[0016] In some embodiments, the counter electrode, the intermediate electrode, and / or the current collector substrate are in a roll form. In some embodiments, an electrode rolling press system is used. In some embodiments, the method is used for a scale-up production.

[0017] This disclosure also provides a system for producing an electrode comprising: a first chamber comprising: an aqueous source comprising lithium and an intermediate electrode. In some embodiments, the intermediate electrode is configured to extract and receive the lithium from the aqueous source to form a lithium-rich intermediate electrode; and a second chamber comprising a current collector substrate. In some embodiments, the lithium-rich intermediate electrode is configured to be transferred from the first chamber to the second chamber. In some embodiments, the lithium from the lithium-rich intermediate electrode is transferred to the current collector substrate to form an electrode for a rechargeable energy device.

[0018] In some embodiments, the aqueous source comprising lithium is brine. In some embodiments, the aqueous source comprising lithium further comprises Na+, K+, Mg2+, Ca2+, B(OH)4, Fe2+, Fe3+, Mn2+, MnO , MnO4, Cl’, SO42’, NH3, NH4+, NH40H, NO2, HN02, NO3’, an alkali metal ions, an alkali earth metal ions, or any combination thereof. In some embodiments, the aqueous source comprising lithium comprises a geological resource. In some embodiments, the aqueous source comprising lithium is pretreated to remove Na+, K+, Mg2+, Ca2+, B(OH)4, Fe2+, Fe3+, Mn2+, MnO42, MnO4, CF, SO42’, NH3, NH4+, NH40H, NO2, HN02, NO3‘, an alkali metal ions, an alkali earth metal ions, or any combination thereof.

[0019] In some embodiments, the extracting and receiving the lithium from the aqueous source is performed by connecting a counter electrode to the intermediate electrode in a circuit, using the aqueous source comprising lithium as an electrolyte. In some embodiments, the lithium from the lithium-rich intermediate electrode is transferred to the current collector substrate by applying an electric potential across the lithium-rich intermediate electrode and the current collector substrate.

[0020] In some embodiments, the intermediate electrode in (i) is substantially free of lithium or is in a de-lithiated state. In some embodiments, the intermediate electrode comprises about 30 at% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode is obtained from recycled lithium-ion battery materials.

[0021] In some embodiments, the intermediate electrode is obtained from black mass produced from shredding of lithium-ion battery materials. In some embodiments, the intermediate electrode comprises iron phosphate, manganese oxide, or nickel manganese cobalt oxide.

[0022] In some embodiments, the intermediate electrode comprises a metal current collector or a carbon current collector. In some embodiments, the intermediate electrode comprises the metal current collector. In some embodiments, the metal current collector comprises copper (Cu), titanium (Ti), aluminum (Al), magnesium (Mg), zinc (Zn), tin (Sn), vanadium oxide (V2Os), orany metal that is capable of forming an alloy with lithium. In some embodiments, the intermediate electrode comprises the carbon current collector. In some embodiments, the carbon current collector comprises graphite.

[0023] In some embodiments, the intermediate electrode is non-reactive with non-lithium components in the aqueous source. In some embodiments, the intermediate electrode is reactive with non-lithium components in the aqueous source. In some embodiments, the first chamber comprises a lithium ion-selective membrane that physically separates the intermediate electrode and a nonaqueous / polymer electrolyte from a positive electrode and the aqueous source. In some embodiments, the second chamber comprises a lithium ion-selective membrane that physically separates the lithium-rich intermediate electrode and an electrolyte from a negative electrode and an aqueous source. In some embodiments, the lithium ion-selective membrane permits lithium ions to selectively flow through.

[0024] In some embodiments, the lithium-rich intermediate electrode comprises lithium iron phosphate (LiFePC , LFP), lithium nickel manganese cobalt oxide (LiNiMnCoCh, NMC), lithium manganate (Li2MnO4, LMO), LiCe, LixMgy, LixAly, LixSiy, or a combination thereof.

[0025] In some embodiments, the intermediate electrode is configured to receive the lithium from the aqueous source by intercalating the lithium in the intermediate electrode. In some embodiments, the lithium-rich intermediate electrode comprises at least 30 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium from the lithium-rich intermediate electrode is transferred to the current collector substrate by delithiating the lithium from the lithium-rich intermediate electrode. In some embodiments, the intercalating and the delithiating are reversible.

[0026] In some embodiments, the current collector substrate comprises copper, copper alloy, aluminum, aluminum alloy, titanium, titanium alloy, nickel, nickel alloy, stainless steel, carbonaceous material, or any combination thereof. In some embodiments, the copper alloy comprises Cu-Ni, Cu-Ti, Cu-Zn, Cu-Al, Cu-Sn, or any combination thereof, the current collector substrate comprises Cu-Ni, Cu-Ti, Cu-Zn, Cu-Al, Cu-Sn, Ni-CO, Al-Mg, Fe-Cr-Ni, or any combination thereof.

[0027] In some embodiments, the current collector substrate comprises carbon, carbon paper, carbon cloth or a metal or noble metal mesh or foil. In some embodiments, the current collector substrate comprises a foil, a mesh, a cloth, or a foam. In some embodiments, the lithium from the lithium-rich intermediate electrode is transferred to the current collector substrate by electrodeposition of the lithium as a layer of lithium metal on the current collector substrate.

[0028] In some embodiments, the positive electrode, the intermediate electrode, and / or the current collector substrate are in a roll form.

[0029] In certain aspects, this disclosure provides a system for manufacturing a lithium metal electrode. The lithium metal electrode can comprise (i) a first widget configured to contact an aqueous source comprising lithium with an intermediate electrode, thereby transferring the lithium to the intermediate electrode to form a lithium-rich intermediate electrode; and (ii) a second widget configured to transfer the lithium from the lithium-rich intermediate electrode to a current collector substrate to form the lithium metal electrode.

[0030] In some embodiments, the aqueous source comprising lithium is brine. In some embodiments, the aqueous source comprising Li+further comprises Na+, K+, Mg2+, Ca2+, B(OH)4, Fe2+, Fe3+, Mn2+, MnO , MnO4, Cl’, SO42’, NH3, NH4+, NH40H, NO2, HN02, NO3’, an alkali metal ions, an alkali earth metal ions, or any combination thereof. In some embodiments, the aqueous source comprising lithium comprises a geological resource. In some embodiments, the aqueous source comprising lithium is pretreated to remove Na+, K+, Mg2+, Ca2+, B(OH)4, Fe2+, Fe3+, Mn2+, MnO42, MnO4, CF, SO42’, NH3, NH4+, NH40H, NO2, HN02, NO3‘, an alkali metal ions, an alkali earth metal ions, or any combination thereof.

[0031] In some embodiments, the first widget comprises a counter electrode. In some embodiments, in the first widget the intermediate electrode is connected with the counter electrode in a circuit, using the aqueous source comprising lithium as an electrolyte.

[0032] In some embodiments, the second widget is configured to apply an electric potential across the lithium-rich intermediate electrode and the current collector substrate.

[0033] In some embodiments, before contacting the aqueous source comprising lithium, the intermediate electrode is substantially free of lithium or is in a de-lithiated state. In some embodiments, the intermediate electrode comprises about 30 atomic % (at%) less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode is obtained from recycled lithium-ion battery materials. In some embodiments, the intermediate electrode is obtained from black mass produced from shredding lithium-ion battery materials.

[0034] In some embodiments, the intermediate electrode comprises iron phosphate (FePO4), manganese oxide (MnO2), or nickel manganese cobalt oxide (NixMnyCoi-x-yO2). In some embodiments, the intermediate electrode comprises iron phosphate (FePO4).

[0035] In some embodiments, the intermediate electrode comprises a metal current collector or a carbon current collector. In some embodiments, the intermediate electrode comprises the metalcurrent collector. In some embodiments, the metal current collector comprises copper (Cu), titanium (Ti), aluminum (Al), magnesium (Mg), zinc (Zn), tin (Sn), vanadium oxide (V2O5), or any metal that is capable of forming an alloy with lithium. In some embodiments, the intermediate electrode comprises the carbon current collector. In some embodiments, the carbon current collector comprises graphite.

[0036] In some embodiments, the first widget further comprises a roll-to-roll production part.

[0037] In some embodiments, the first widget operates at temperatures up to about 95°C.

[0038] In some embodiments, the lithium-rich intermediate electrode comprises lithium iron phosphate (LiFePCU, LFP), lithium manganese oxide (LiMn2O4 spinel, or Li2MnO3-based lithium-rich layered materials, LMR-NMC), lithium nickel manganese cobalt oxide (LiNiMnCoCh or NMC), lithium manganate (Li2MnO4, LMO), LiCe, LixMgy, LixAly, LixSiy, or a combination thereof.

[0039] In some embodiments, the lithium-rich intermediate electrode comprises lithium iron phosphate (LiFePC , LFP).

[0040] In some embodiments, the first widget is configured to transfer the lithium from the aqueous source to the intermediate electrode by intercalating the lithium in the intermediate electrode to form the lithium-rich intermediate electrode.

[0041] In some embodiments, wherein the lithium-rich intermediate electrode comprises at least 30 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode operates as a lithium ink.

[0042] In some embodiments, the second widget is configured to transfer the lithium from the lithium-rich intermediate electrode to the current collector substrate by delithiating the lithium- rich intermediate electrode. In some embodiments, the intercalating and the delithiating are reversible.

[0043] In some embodiments, the current collector substrate comprises copper, copper alloy, aluminum, aluminum alloy, titanium, titanium alloy, nickel, nickel alloy, stainless steel, carbonaceous material, or any combination thereof. In some embodiments, the current collector substrate comprises Cu. In some embodiments, the copper alloy comprises Cu-Ni, Cu-Ti, Cu-Zn, Cu-Al, Cu-Sn, or any combination thereof, the current collector substrate comprises Cu-Ni, Cu- Ti, Cu-Zn, Cu-Al, Cu-Sn, Ni-CO, Al -Mg, Fe-Cr-Ni, or any combination thereof.

[0044] In some embodiments, the current collector substrate comprises carbon, carbon paper, carbon cloth or a metal or noble metal mesh or foil. In some embodiments, the current collector substrate comprises a foil, a mesh, a cloth, or a foam.

[0045] In some embodiments, an electrical connection to the lithium-rich intermediate electrode is made via copper, copper alloy, aluminum, aluminum alloy, titanium, titanium alloy, nickel, nickel alloy, stainless steel, carbonaceous material, or any combination thereof.

[0046] In some embodiments, the transferring of the lithium from the lithium-rich intermediate electrode to the current collector substrate comprises electrodeposition of the lithium as a layer of lithium metal on the current collector substrate.

[0047] In some embodiments, the lithium is electrodeposited as a layer of lithium metal at least 1 micrometer (pm) thickness of a layer / min.

[0048] In some embodiments, the electrodepositing comprises coating or printing the electrode ink on the current collector substrate.

[0049] In some embodiments, the second widget operates at a temperature of about 10°C to about 150°C. In some embodiments, the second widget operates at a pressure of about 0.05 MPa to about 15 MPa. In some embodiments, the second widget operates at about 0.1 mA / cm2to about 50 mA / cm2.

[0050] In some embodiments, the second widget comprises an electrolyte. In some embodiments, the electrolyte comprises (a) 1,3 -di oxolane (DOL): 1,2-dimethoxy ethane (DME), 1 M lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), 1% LiNCh, (b) 2EC (ethylene carbonate): 3 EMC (ethyl methyl carbonate), 1 M LiTFSI, (c) tetraethylene glycol dimethyl ether (G4), 1 M LiNCE, or (d) di ethylene glycol dimethyl ether (G2), 1 M LiNCh.

[0051] In some embodiments, a boiling point of the electrolyte ranges from about 70°C to about 290°C. In some embodiments, the electrolyte is non-volatile.

[0052] In some embodiments, the second widget is configured to provide a separator between the lithium rich intermediate electrode and the current collector substrate.

[0053] In some embodiments, the separator comprises a lithium ion-selective membrane permitting lithium ions to selectively flow through.

[0054] In some embodiments, the lithium ion-selective membrane comprises a single layer or multiple layers. In some embodiments, the lithium ion-selective membrane comprises glass fiber, polyester, polyethylene, polypropylene, polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), and a combination thereof.

[0055] In some embodiments, the lithium ion-selective membrane comprises hydrophobic polymers.

[0056] In some embodiments, the lithium ion-selective membrane comprises lithium-ion conductive channels.

[0057] In some embodiments, a columbic efficiency of the system ranges from about 60% to about 100%. In some embodiments, a columbic efficiency of the system ranges from about 80% to about 100%.

[0058] In some embodiments, the second widget is configured to produce a two-sided lithium metal electrode.

[0059] In some embodiments, the lithium metal electrode is a battery-ready electrode.

[0060] In some embodiments, a surface roughness of the lithium metal electrode is less than about 3.0 pm. In some embodiments, a surface roughness of the lithium metal electrode is less than about 1.0 pm.

[0061] In some embodiments, a purity of the lithium metal electrode is higher than about 98%. In some embodiments, a purity of the lithium metal electrode is higher than about 99.9%.

[0062] In some embodiments, a deposition efficiency of the second widget is higher than about 95%. In some embodiments, a deposition efficiency of the second widget is higher than about 98%. In some embodiments, the lithium-rich intermediate electrode is delithiated at the second widget and returned to the first widget.

[0063] In some embodiments, the lithium metal electrode is treated by refining or post processes. In some embodiments, the refining or post processes comprise cleaning, heating, calendaring, or applying pressure on the electrode. In some embodiments, the refining or post processes comprise applying heat to the electrode at a temperature below about 150°C. In some embodiments, the refining or post processes comprise applying pressure on the electrode at most 5 MPa.

[0064] In some embodiments, the counter electrode, the intermediate electrode, and / or the current collector substrate are in a roll form.

[0065] In some embodiments, the second widget further comprises a roll-to-roll production part.

[0066] In some embodiments, the system is used for a scale-up production.

[0067] In some embodiments, the system is configured to repeatedly produce a lithium metal electrode from one lithium rich intermediate electrode.

[0068] Additional aspects and advantages of the present disclosure will become readily apparent to those skilled in this art from the following detailed description, wherein only illustrative embodiments of the present disclosure are shown and described. As will be realized, the present disclosure is capable of other and different embodiments, and its several details are capable of modifications in various obvious respects, all without departing from the disclosure.Accordingly, the drawings and description are to be regarded as illustrative in nature, and not as restrictive.INCORPORATION BY REFERENCE

[0069] All publications, patents, and patent applications mentioned in this specification are herein incorporated by reference to the same extent as if each individual publication, patent, or patent application was specifically and individually indicated to be incorporated by reference.BRIEF DESCRIPTION OF THE DRAWINGS

[0070] The novel features of the disclosure are set forth with particularity in the appended claims. A better understanding of the features and advantages of the present disclosure will be obtained by reference to the following detailed description that sets forth illustrative embodiments, in which the principles of the disclosure are utilized, and the accompanying drawings (“FIGURE.” or “FIGURES.” herein) of which:

[0071] FIG. 1 shows a block diagram of the overall process of lithium extraction and preparation of lithium metal electrode, in accordance with aspects of the present disclosure.

[0072] FIG. 2 shows a diagram of a system comprising an intermediate electrode, in accordance with aspects of the present disclosure.

[0073] FIG. 3 shows a diagram of a system with a two-chamber design, in accordance with aspects of the present disclosure.

[0074] FIG. 4 shows the capacities and voltages of an intermediate electrode used to produce a lithium electrode, in accordance with aspects of the present disclosure. In reaction 1, the lithium from the lithium rich feedstock is absorbed into the intermediate electrode. In reaction 2, the lithium is removed from the intermediate electrode and plated as a lithium metal electrode onto a copper current collector.

[0075] FIG. 5 shows an optional upgrading / refining step of the electrodeposited lithium, in accordance with aspects of the present disclosure.

[0076] FIG. 6 shows a cyclic voltammogram of LiFePCf electrode in a mixed solution of Li2SO4 and NaCl versus in a pure NaCl solution, in accordance with aspects of the present disclosure.

[0077] FIG. 7 shows cyclic voltammograms of the intercalation of lithium ions into the framework of the cathode material - FP and LFP - during charging and the deintercalation, in accordance with aspects of the present disclosure.

[0078] FIG. 8A-FIG. 8D show cyclic voltammograms of LFP electrode working in various brines, in accordance with aspects of the present disclosure.

[0079] FIG. 9 shows comparison of the surface roughness of a commercial lithium metal electrode and a lithium metal electrode produced by methods and systems disclosed herein, in accordance with aspects of the present disclosure.

[0080] FIG. 10 shows measurements of surface roughness of lithium metal layer prepared by methods and systems disclosed herein, in accordance with aspects of the present disclosure.

[0081] FIG. 11 shows measurements of nodule size of lithium metal layer prepared by methods and systems disclosed herein, in accordance with aspects of the present disclosure.

[0082] FIG. 12 shows the experimental results for a long term cycle performance of a full cell, in accordance with aspects of the present disclosure.

[0083] FIG. 13 shows a flow chart of the process for manufacturing a lithium metal electrode, in accordance with aspects of the present disclosure.

[0084] FIG. 14 shows a computer system, in accordance with aspects of the present disclosure.DETAILED DESCRIPTION

[0085] Lithium can be extracted from various sources. Two primary sources include salt-flat brines and mineral ores, such as spodumene. Salt-flat brines can be found in saltwater lakes and can contain high concentrations of lithium. Mineral ores, on the other hand, can be found in rock formations that contain lithium-bearing minerals. The process of extracting lithium from these sources can be complex and involves multiple stages. In the case of salt-flat brines, the extraction process can begin by pumping the brine into large evaporation ponds, where solar evaporation can be used to evaporate water over several months. As the water evaporates, lithium-rich salts can gradually concentrate. The concentrated brine can then be further processed using various methods, including chemical precipitation and absorption (e.g., using ion exchange resins), to isolate lithium carbonate or lithium hydroxide. For mineral ores like spodumene, the extraction process can start with mining and crushing the ore, followed by roasting it at high temperatures. This process can convert the lithium-bearing minerals into water-soluble compounds. The roasted ore can then be subjected to acid leaching, where the lithium is extracted and converted into lithium carbonate. Once lithium carbonate is obtained, it can be further processed intolithium chloride (LiCl) for use in high-temperature molten salt electrolysis. This method can involve using LiCl as a feedstock for the electrolysis process, where lithium metal is deposited onto a cathode. This electrolysis process can be energy-intensive and can require operating at high temperatures.

[0086] Some methods of preparing lithium metal electrodes can involve extrusion or thin film high vacuum vapor deposition of lithium metal. Extrusion can involve forcing lithium metal through a die, which can result in a desired shape for the electrode. Thin film high vacuum vapor deposition, on the other hand, can involve depositing thin layers of lithium metal onto a substrate under high vacuum conditions. Both of these electrode preparation methods face challenges in achieving high purity and low defect electrodes. The presence of impurities or defects can impact the performance and lifespan of lithium-based batteries. Additionally, these methods are often expensive, limiting the scalability and affordability of lithium-based products.

[0087] There have been considerable efforts to develop alternative and more efficient approaches. These advancements aim to make lithium extraction and electrode production more cost-effective, environmentally friendly, and accessible for widespread use. The improvement of lithium extraction and the preparation of lithium metal electrodes are crucial for the advancement of energy storage technologies, as they can contribute to the development of more efficient and sustainable lithium-based products that will help shape the future of transportation and renewable energy systems.

[0088] In some aspects, provided herein are methods and systems for preparing lithium metal electrodes for rechargeable energy devices in a continuous two-step process. In certain aspects, this disclosure provides a two-step process for selective electrochemical extraction of lithium from an aqueous source comprising lithium, followed by electrochemical plating of lithium metal for use as a Li-metal battery electrode.

[0089] A further aspect of the present disclosure relates to the utilization of used battery electrodes as shown in FIG. 1. In some embodiments, the used battery electrodes comprise a delithiated electrode or black mass. In some embodiments, the delithiated electrode is used as a Li host disposed of in an aqueous source comprising lithium. In some embodiments, the used electrode is cycled through two chambers, first selectively extracting lithium from an aqueous source, drying the electrode, and transferring the electrode to an electrodeposition chamber where the lithium is extracted and plated as a battery-ready lithium metal electrode. In some embodiments, the electrode that is delithiated in the electrodeposition chamber can be reused as the Li host in the aqueous source comprising lithium.

[0090] The term “black mass” as used herein can refer to a composite material primarily obtained from the recycling of end-of-life batteries and battery production scrap. The black mass can comprise various metals including lithium, nickel, cobalt, manganese, and copper, rendering it a significant resource for raw material recovery. In some embodiments, the particle size of the black mass can be at least 1 pm, 2 pm, 3 pm, 4 pm, 5 pm, 6 pm, 7 pm, 8 pm, 9 pm, 10 pm, 50 pm, 100 pm, 150 pm, 200 pm, 250 pm, 300 pm, 350 pm, or 400 pm. In some embodiments, the particle size of the black mass can be at most 1 pm, 2 pm, 3 pm, 4 pm, 5 pm, 6 pm, 7 pm, 8 pm, 9 pm, 10 pm, 50 pm, 100 pm, 150 pm, 200 pm, 250 pm, 300 pm, 350 pm, or 400 pm. The size and the composition can depend on an outcome of several processes such as discharging, shredding, and calcination. The black mass can comprise materials derived during various stages of battery manufacturing. In some embodiments, cathode active material scraps are generated during the manufacturing process of the cathode active material. In some embodiments, the production and processing of the cathode foil can produce cathode scraps. In some embodiments, scraps can be formed during the lamination process of the cathode, the anode plate, and the separator. In some embodiments, scraps can be generated during the battery cell assembly process. In some embodiments, scraps can be formed during the modularizing process of the cells. In some embodiments, black mass comprises Ni, Co, Li, Cu, Al, Mn, F, Fe, Mg, K, or P.

[0091] In some cases, black mass can be subjected to extracting and refining valuable metals such as lithium, nickel, cobalt, and manganese. The extracting and refining processes can include several phases. The first phase involves mixing the black mass with sulfuric acid. The mixture of sulfuric acid and black mass forms a leachate, dissolving the valuable metals. This mixture can undergo high-pressure oxygen leaching, followed by filtration to remove undissolved solids and impurities, leaving purified leachate enriched with valuable metals.

[0092] In some embodiments, the purification of the leachate can be followed by a series of extraction and refining steps aimed at isolating and purifying the valuable metals. The process involves introducing the leachate into an extraction system wherein an extractant is added. The extractant can have the property of selectively binding with the metals, effectively separating them from the leachate. In some embodiments, subsequent to the extraction process, the mixture undergoes a cleaning process designed to remove any residual impurities. In some embodiments, following the cleaning process, a reverse extraction procedure can be employed wherein the bound metals are stripped from the extractant. In some embodiments, a regeneration process can be initiated, serving to further refine the separated metals.

[0093] The next stage can involve the concentration of these valuable metals. In some embodiments, the metal-enriched solution can be introduced into an evaporator and heat exchanger system, where the water content is significantly reduced, increasing the concentration of the metals. The concentrated solution can be introduced into a crystallizer where the metals crystallize out of the solution. The crystallized metals can be separated using a centrifuge and dried in a dryer.

[0094] In some embodiments, the phase can involve the transformation of the lithium sulfate solution into lithium carbonate powder. The lithium sulfate solution can be subjected to a filter press to remove impurities. The filtered solution can be introduced to a carbonation tank where a carbonating agent is added. In some embodiments, the carbonating agent comprises carbon dioxide. The lithium carbonate can be sent to a centrifuge for further purification. The purified lithium carbonate can be heated to remove any remaining water content and prepared as a fine powder.Lithium Resource

[0095] In some aspects, the present disclosure provides systems and methods of extracting lithium from a lithium resource. A lithium resource can be a natural resource, e.g., a geological resource comprising ore, minerals, or brine, or seawater. A lithium resource can be a salar brine, a salt-lake brine, an oil-field brine, a bromine-plan tail brine, a geothermal brine, a fracking brine, a leachate from mining, an effluent from an industrial process (e.g., from a battery recycling plant), or a combination thereof. The term “lithium resource” as used herein means an aqueous source comprising lithium.

[0096] In some embodiments, the lithium resource comprises an aqueous solution of metal salts comprising (i) a lithium salt and (ii) a sodium salt, a magnesium salt, a calcium salt, a potassium salt, or any combination thereof. In some embodiments, the lithium resource comprises an aqueous salt solution. In some embodiments, the lithium resource comprises sodium, potassium, magnesium, calcium, boron, chlorine, SCU2', nitrogen, an alkali metal, an alkali earth metal, or any combination thereof. In some embodiments, the magnesium salt comprises MgCh. In some embodiments, the sodium salt comprises NaCl. In some embodiments, the lithium resource comprises LiCl, Li2SO4, or both.

[0097] In some embodiments, a ratio of magnesium to lithium in the lithium resource is at least 0, 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 20, 30, 40, 50, 60, 70, 80, 90, 100, 200, 300, 400, 500, 600, 700, 800, 900, or 1000 on a molar basis. In some embodiments, a ratio of magnesium to lithium in the lithium resource is at most 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 20, 30, 40, 50, 60, 70, 80, 90, 100, 200,300, 400, 500, 600, 700, 800, 900, or 1000 on a molar basis. In some embodiments, a ratio of magnesium to lithium in the lithium resource is at least 0, 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 20, 30, 40, 50, 60, 70, 80, 90, 100, 200, 300, 400, 500, 600, 700, 800, 900, or 1000 on a mass basis. In some embodiments, a ratio of magnesium to lithium in the lithium resource is at most 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 20, 30, 40, 50, 60, 70, 80, 90, 100, 200, 300, 400, 500, 600, 700, 800, 900, or 1000 on a mass basis.

[0098] In some embodiments, the lithium resource comprises a total dissolved solid concentration of at least 100, 200, 300, 400, 500, 600, 700, 800, 900, 1000, 2000, 3000, 4000, 5000, 6000, 7000, 8000, 9000, 10000, 20000, 30000, 40000, 50000, 60000, 70000, 80000, 90000, or 100000 mg / L. In some embodiments, the lithium resource comprises a total dissolved solid concentration of at most 100, 200, 300, 400, 500, 600, 700, 800, 900, 1000, 2000, 3000, 4000, 5000, 6000, 7000, 8000, 9000, 10000, 20000, 30000, 40000, 50000, 60000, 70000, 80000, 90000, or 100000 mg / L.

[0099] In some embodiments, the lithium resource can be pretreated to remove a metal cation. In some embodiments, the metal cation comprises magnesium, calcium, sodium, potassium, iron, or any combination thereof. In some embodiments, the metal cation can be removed by adsorption, extraction, absorption, electrodialysis, precipitation, nanofiltration, solvent extraction, or any combination thereof. In some embodiments, the adsorption or the extraction comprises binding the metal cation to a coordination compound. In some embodiments, the absorption can be performed by contacting the lithium resource with lithium-manganese oxide, titanium oxide, aluminum hydroxide, iron phosphate, clay minerals, zeolite, zirconium phosphate, tin antimonate, antimony oxide, tantalum oxide, niobium oxide, or any combination thereof.

[0100] In some embodiments, lithium can be extracted from a geological resource, such as clay and / or ore. In some embodiments, the geological resource can comprise a lithium mineral (e.g., LiAlSi2Oe). The geological resource can be treated with sulfuric acid to obtain solution comprising Li2SO4. The Li2SO4 can be crystallized or further treated with a base to obtain LiOH (e.g., by adding Ca(OH)2) or Li2CO3 (e.g., by adding ISfeCCh). In some embodiments, CaSCU can be added to the geological resource. In some embodiments, the geological resource can be baked at high temperature. In some embodiments, LiSCL can be extracted using water to obtain an aqueous solution. In some embodiments, the aqueous solution can be concentrated to obtain Li2SO4 as a crystal.

[0101] In some embodiments, the lithium resource or the electrolyte comprises an additive, wherein the additive is configured to bind with lithium ions in the lithium resource preferentiallyover the lithium ions binding with water. In some embodiments, the lithium resource comprises an anion with a chemical structure of (RS(O)2)2N‘, where R is a substituent selected from the group of alkyl, perfluorinated alkyl, partially fluorinated alkyl, aryl, perfluorinated aryl, partially fluorinated aryl, and combinations thereof.

[0102] In some embodiments, the lithium resource comprises at least 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 20, 30, 40, 50, 60, 70, 80, 90, 100, 200, 300, 400, 500, 600, 700, 800, 900, 1000, 2000, 3000, 4000, 5000, 6000, 7000, 8000, 9000, 10000, 20000, 30000, 40000, or 50000 mg / L of lithium. In some embodiments, the lithium resource comprises at most 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 20, 30, 40, 50, 60, 70, 80, 90, 100, 200, 300, 400, 500, 600, 700, 800, 900, 1000, 2000, 3000, 4000, 5000, 6000, 7000, 8000, 9000, 10000, 20000, 30000, 40000, or 50000 mg / L of lithium.PRETREAMENT OF LITHIUM RESOURCE

[0103] In certain aspects, the lithium resource can be pretreated by various methods. The methods include, but not limited to dilution, concentration, filtration, nanofiltration, absorption or extraction using organic molecules or inorganic sorbents, electrodialysis using a membrane, concentration and precipitation, solvent extraction, pH adjustment, or any combination thereof. These methods can be used individually or in combination depending on the specific requirements of the lithium resource being treated.

[0104] In some embodiments, an aqueous source comprising lithium can comprise a pretreated lithium resource. In some embodiments, an aqueous source comprising lithium can comprise a non-pretreated lithium resource.

[0105] In some embodiments, a lithium resource can be limed. Liming can adjust the pH, reduce the concentration of non-lithium components, precipitate phosphorus, precipitate non-lithium metals such as magnesium, or a combination thereof. Precipitates can be separated from the lithium resource by, e.g., solid-liquid separation.

[0106] In some embodiments, a lithium resource can be concentrated. This can be accomplished through various methods such as reverse osmosis or boiling to eliminate water from the resource. In some embodiments, pretreatment approaches may include processes for removing organic molecules, eradicating hydrogen sulfide, precipitating iron, flocculation, or filtering to remove solids. These methods can be used individually or in combination depending on the specific requirements of the lithium resource being treated.

[0107] In some embodiments, the pH adjustment comprises adding an acid, a base, a buffer, or any combination thereof.

[0108] In some embodiments, the pretreatment removes magnesium ions in the lithium resource. The extraction and separation of lithium ions from magnesium ions in the lithium resource comprising brine solutions can be achieved through several approaches comprising the use of specially engineered solvents or absorbents. In some embodiments, lithium-selective sorbents can selectively trap lithium ions due to their unique structural properties. These sorbents often derive from materials like titanium dioxide or aluminum oxide. Organic solvents, such as tributyl phosphate, can also be employed due to their capability to dissolve lithium salts selectively, while leaving other salts like those of magnesium intact. In some embodiments, electrical processes can be used for the selective extraction of lithium ions. Electrodialysis as a membrane process promotes the transportation of ions through an ion-exchange membrane under the influence of an electric potential. In some cases, membranes specifically designed to favor lithium ions can be used to enhance the selectivity of lithium extraction. In some embodiments, capacitive deionization can be used for the separation of lithium ions from magnesium ions in the lithium resource. For capacitive deionization, an electric field can be applied to remove ions from the brine. Here, electrodes with a preferential affinity for lithium ions can be utilized. In some embodiments, membrane-based methods offer other strategies for the efficient separation of lithium from magnesium ions. In some embodiments, nanofiltration uses specially designed membranes with particular pore sizes and surface properties that selectively allow lithium ions to pass while rejecting larger or differently charged ions like magnesium. In some embodiments, reverse osmosis, although not as selective as nanofiltration, can effectively reduce the overall salinity of the brine, making subsequent lithium extraction processes more efficient. In some embodiments, membrane distillation can be used in tandem with other processes to enhance lithium recovery, despite it typically not being selective for lithium over magnesium. In some embodiments, after pretreatment for separation of lithium ions from magnesium ions in the lithium resource, a molar ratio of Li+ / Mg2+is at least 10, 20, 30, 40, 50, 60, 70, 80, 90, 100, 120, 140, 160, 180, or 200. In some embodiments, after pretreatment for separation of lithium ions from magnesium ions in the lithium resource, a molar ratio of Li+ / Mg2+is at most 50, 60, 80, 100, 120, 140, 160, 180, 200, 250, 300, 350, 400, or 500.

[0109] In some embodiments, the pretreatment involves heating up the lithium resource comprising brine up to 80°C. In some embodiments, the lithium resource can be heated up to at least 50°C, 55°C, 60°C, 65°C, 70°C, 75°C, or 80°C. In some embodiments, the lithium resource can be heated up to at most 50°C, 55°C, 60°C, 65°C, 70°C, 75°C, or 80°C.

[0110] In some embodiments, the lithium resource can be utilized to produce lithium hydroxide, lithium chloride, lithium carbonate, or a combination thereof. This production can result in these compounds existing within an aqueous solution. Subsequently, these generated compounds can be dried to form a solid. This dried lithium hydroxide, lithium chloride, or lithium carbonate can then be dissolved in water, yielding an aqueous solution rich in lithium ions. This lithium-ion enriched solution can be used for the preparation of a negative electrode comprising lithium metal.[oni] In some embodiments, the pretreating can be performed using a system. The system can comprise a pump configured to pressurize an input flow of the lithium resource. The lithium resource can be pressurized into one or more vessels comprising one or more membranes and one or more columns. The one or more membrane and / or the one or more columns can be configured to selectively transport lithium over other cations, or a monovalent anion over other anions. In some embodiments, the one or more membrane and / or the one or more columns can be configured to concentrate lithium by removing water, e.g., by reverse osmosis. The lithium resource can be treated to adjust its pH, filter solids, precipitate non-lithium salts, or any combination thereof before inputting to the system.

[0112] In some embodiments, the system is configured to adjust the pH of the lithium resource. In some embodiments, the pH of the lithium resource can be adjusted to at least 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, or 14. In some embodiments, the pH of the lithium resource can be adjusted to at most 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, or 14.

[0113] In some embodiments, a volume of the lithium resource comprising brine that the system can daily process is at least 10 m3, 20 m3, 30 m3, 40 m3, 50 m3, 100 m3, 150 m3, 200 m3, 250 m3, 300 m3, 350 m3, 400 m3, 450 m3, 500 m3, 1000 m3, 2000 m3, 4000 m3, 6000 m3, 8000 m3, 10000 m3, 12000 m3, 14000 m3, 16000 m3, 18000 m3, 20000 m3, 22000 m3, 24000 m3, 26000 m3, 28000 m3, or 30000 m3. In some embodiments, a volume of the lithium resource comprising brine that the system can daily process is at most 100 m3, 150 m3, 200 m3, 250 m3, 300 m3, 350 m3, 400 m3, 450 m3, 500 m3, 1000 m3, 2000 m3, 4000 m3, 6000 m3, 8000 m3, 10000 m3, 12000 m3, 14000 m3, 16000 m3, 18000 m3, 20000 m3, 22000 m3, 24000 m3, 26000 m3, 28000 m3, 30000 m3, 40000 m3, 45000 m3, 50000 m3, 60000 m3, 70000 m3, 80000 m3, 90000 m3, or 100000

[0114] The output flow from the system can have a lithium purity of at least 50, 60, 70, 80, 85, 90, 91, 92, 93, 94, 95, 96, 97, 98, or 99 percent on a metals basis. The output flow from the system can have a lithium purity of at most 50, 60, 70, 80, 85, 90, 91, 92, 93, 94, 95, 96, 97, 98,99, or 99.9 percent on a metals basis. In some embodiments, the system recovers at least 60, 70, 80, 85, 90, 91, 92, 93, 94, 95, 96, 97, 98, or 99 percent of lithium in the lithium resource. In some embodiments, the system recovers at most 60, 70, 80, 85, 90, 91, 92, 93, 94, 95, 96, 97, 98, or 99 percent of lithium in the lithium resource.

[0115] In some embodiments, the system comprises a filter. The filter can be used to remove solids, organics, or descaling the lithium resource. In some embodiments, the system can comprise a water softener. In some embodiments, the system can be configured to remove hydrogen sulfide from the lithium resource.

[0116] In some embodiments, the system can comprise an electrodialyzer. The electrodialyzer can be configured to increase a concentration of lithium in a solution and / or to extract lithium from a lithium resource. The electrodialyzer can be configured to increase a concentration of lithium chloride, lithium hydroxide, or lithium carbonate in the lithium resource.INTERMEDIATE ELECTRODE

[0117] In some embodiments, as shown in FIG. 2, in the process of lithium extraction of brine, the intermediate electrode can be used as the electrode or current collector for depositing lithium (e.g., a de-lithiated cathode). In another embodiment, as shown in FIG. 2, the intermediate electrode can be used as a lithium source for transferring lithium to a current collector substrate. In some cases, the intermediate electrode can be transformed as a temporary reservoir of lithium to form a lithium-rich intermediate electrode, which is subsequently used to form an electrode for a rechargeable energy device. In this process, the lithium ions from the lithium-rich intermediate electrode are transferred onto a current collector substrate. The transfer results in the formation of a lithium-based electrode, ready to be incorporated into a rechargeable energy device, such as a lithium-ion battery.

[0118] In some embodiments, a current collector substrate may have a thickness of at least 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 20, 30, 40, 50, 60, 70, 80, 90, 100, 200, 300, 400, 500, 600, 700, 800, 900, or 1000 pm. In some embodiments, a current collector substrate may have a thickness of at most 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 20, 30, 40, 50, 60, 70, 80, 90, 100, 200, 300, 400, 500, 600, 700, 800, 900, or 1000 pm. In some embodiments, a current collector substrate comprises copper, stainless steel, aluminum, nickel, titanium, sintered carbon, copper or stainless steel that is surface-treated with carbon, nickel, titanium or silver, and aluminum-cadmium alloys. In some embodiments, a current collector substrate comprises fine irregularities on surfaces thereof so as to enhance adhesive strength of the electrode current collector substrate to the electrode active material.

[0119] In some embodiments, a current collector substrate can comprise various forms including films, sheets, foils, nets, porous structures, foams, and non-woven fabrics. In some embodiments, a current collector substrate comprises carbon, carbon paper, carbon cloth or a metal or noble metal mesh or foil. Derived from the carbonization process of a polymeric precursor such as polyacrylonitrile (PAN) or rayon, carbon cloth is composed of a complex network of pure carbon fibers. High electrical conductivity, high thermal stability, and mechanical strength define the attributes of carbon cloth, making it a suitable material for battery applications. Carbon cloth has resistance to chemical corrosion. High surface area of carbon cloth can promote efficient electron transfer, contributing to high energy and power densities in the lithium batteries. Carbon cloth has porous structure to enhance electrolyte penetration, thereby further increasing the performance metrics of the battery. In addition, carbon cloth offers its light weight and flexibility. Adaptable nature of carbon cloth enables its use in a diverse range of battery configurations, including those requiring bendability or shape conformity.

[0120] In some embodiments, the intermediate electrode can have high porosity to provide large surface area for lithium interaction and adsorption. In some embodiments, the material of the intermediate electrode comprises porous carbon or porous metal oxides, which offer large internal surface areas. In some embodiments, the intermediate electrode can have a suitable lattice structure that can accommodate lithium ions, comprising intercalation compounds, such as graphite or transition metal oxides. The crystal structure of these materials provides interstitial spaces where lithium ions can reside, facilitating lithium uptake. In some embodiments, the intermediate electrode have good electronic conductivity to enable efficient charge transfer during lithium adsorption and desorption processes. In some embodiments, the intermediate electrode can be chemically stable in the aqueous source and during lithium transfer processes to prevent degradation and ensure efficient lithium transfer over repeated cycles. In some embodiments, the intermediate electrode can have the mechanical robustness to withstand the stress induced during the lithium uptake and release, without undergoing significant volume changes that could compromise the structural integrity of the electrode. In some embodiments, the intermediate electrode also exhibits electrochemical stability in water. When a potential is applied to intercalate the intermediate electrode with lithium, the electrode material can be chosen such that it prevents the electrolysis of water and the subsequent evolution of hydrogen (H2) or oxygen (O2) gases.

[0121] In some embodiments, the intermediate electrode can be a negative electrode. In some embodiments, the intermediate electrode is substantially free of lithium. In some embodiments,the intermediate electrode is in a de-lithiated state. In some embodiments, the intermediate electrode comprises 60 atomic % (at%), 58 at%, 56 at%, 54 at%, 52 at%, 50 at%, 48 at%, 46 at%, 44 at%, 42 at%, 40 at%, 38 at%, 36 at%, 34 at%, 32 at%, 30 at%, 28 at%, 26 at%, 24 at%, 22 at%, 20 at%, 18 at%, 16 at%, 14 at%, 12 at%, or 10 at% less than a maximum amount of lithium that can be present, before contacting with an aqueous source comprising lithium. In some embodiments, the intermediate electrode comprises about 60 atomic % (at%), about 58 at%, about 56 at%, about 54 at%, about 52 at%, about 50 at%, about 48 at%, about 46 at%, about 44 at%, about 42 at%, about 40 at%, about 38 at%, about 36 at%, about 34 at%, about 32 at%, about 30 at%, about 28 at%, about 26 at%, about 24 at%, about 22 at%, about 20 at%, about 18 at%, about 16 at%, about 14 at%, about 12 at%, or about 10 at% less than a maximum amount of lithium that can be present, before contacting with an aqueous source comprising lithium. In some embodiments, the intermediate electrode comprises about 60 at% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 58 at% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 56 at% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 54 at% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 52 at% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 50 at% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 48 at% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 46 at% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 44 at% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 42 at% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 40 at% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 38 at% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 36 at% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 34 at% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 32 at% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrodecomprises about 30 at% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 28 at% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 26 at% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 24 at% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 22 at% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 20 at% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 18 at% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 16 at% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 14 at% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 12 at% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 10 at% less than a maximum amount of lithium that can be present.

[0122] In some embodiments, the intermediate electrode comprises 60 mole%, 58 mole%, 56 mole%, 54 mole%, 52 mole%, 50 mole%, 48 mole%, 46 mole%, 44 mole%, 42 mole%, 40 mole%, 38 mole%, 36 mole%, 34 mole%, 32 mole%, 30 mole%, 28 mole%, 26 mole%, 24 mole%, 22 mole%, 20 mole%, 18 mole%, 16 mole%, 14 mole%, 12 mole%, or 10 mole% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 60 mole%, about 58 mole%, about 56 mole%, about 54 mole%, about 52 mole%, about 50 mole%, about 48 mole%, about 46 mole%, about 44 mole%, about 42 mole%, about 40 mole%, about 38 mole%, about 36 mole%, about 34 mole%, about 32 mole%, about 30 mole%, about 28 mole%, about 26 mole%, about 24 mole%, about 22 mole%, about 20 mole%, about 18 mole%, about 16 mole%, about 14 mole%, about 12 mole%, or about 10 mole% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 60 mole% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 58 mole% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 56 mole% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 54 mole% less than a maximum amount of lithium that can be present. In some embodiments, the intermediateelectrode comprises about 52 mole% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 50 mole% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 48 mole% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 46 mole% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 44 mole% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 42 mole% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 40 mole% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 38 mole% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 36 mole% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 34 mole% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 32 mole% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 30 mole% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 28 mole% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 26 mole% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 24 mole% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 22 mole% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 20 mole% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 18 mole% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 16 mole% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 14 mole% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 12 mole% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises about 10 mole% less than a maximum amount of lithium that can be present.

[0123] In some embodiments, the intermediate electrode comprises at least 60 at%, 58 at%, 56 at%, 54 at%, 52 at%, 50 at%, 48 at%, 46 at%, 44 at%, 42 at%, 40 at%, 38 at%, 36 at%, 34 at%, 32 at%, 30 at%, 28 at%, 26 at%, 24 at%, 22 at%, 20 at%, 18 at%, 16 at%, 14 at%, 12 at%, or 10 at% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 60 at% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 58 at% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 56 at% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 54 at% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 52 at% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 50 at% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 48 at% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 46 at% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 44 at% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 42 at% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 40 at% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 38 at% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 36 at% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 34 at% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 32 at% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 30 at% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 28 at% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 26 at% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 24 at% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 22 at% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 20 at% of a maximum amount of lithium that can bepresent. In some embodiments, the intermediate electrode comprises at least 18 at% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 16 at% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 14 at% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 12 at% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 10 at% of a maximum amount of lithium that can be present.

[0124] In some embodiments, the intermediate electrode comprises at least 60 mole%, 58 mole%, 56 mole%, 54 mole%, 52 mole%, 50 mole%, 48 mole%, 46 mole%, 44 mole%, 42 mole%, 40 mole%, 38 mole%, 36 mole%, 34 mole%, 32 mole%, 30 mole%, 28 mole%, 26 mole%, 24 mole%, 22 mole%, 20 mole%, 18 mole%, 16 mole%, 14 mole%, 12 mole%, or 10 mole% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 60 mole% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 58 mole% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 56 mole% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 54 mole% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 52 mole% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 50 mole% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 48 mole% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 46 mole% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 44 mole% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 42 mole% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 40 mole% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 38 mole% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 36 mole% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 34 mole% of a maximum amount of lithium that can be present. In some embodiments, theintermediate electrode comprises at least 32 mole% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 30 mole% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 28 mole% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 26 mole% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 24 mole% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 22 mole% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 20 mole% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 18 mole% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 16 mole% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 14 mole% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 12 mole% of a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 10 mole% of a maximum amount of lithium that can be present.

[0125] In some embodiments, the intermediate electrode is obtained from recycled lithium-ion battery materials. In some embodiments, the intermediate electrode comprises black mass produced from the shredding of lithium-ion battery materials. In some embodiments, the black mass comprises the shredding de-lithiated lithium-ion battery materials comprising lithium iron phosphate (LFP), lithium nickel manganese cobalt oxide (NMC) lithium-ion batteries, or Li2MnO4 (LMO). In some embodiments, the intermediate electrode comprises iron phosphate, manganese oxide, or nickel manganese cobalt oxide.

[0126] In some embodiments, the intermediate electrode comprises lithium iron phosphate (LFP). LFP can have a high selectivity for lithium extraction due to its specific crystal structure. The olivine structure of LFP contains distinct pathways (tunnels) for lithium ions to move in and out, while largely blocking the movement of other types of ions. In this way, LFP can be said to have a "structural selectivity" for lithium ions, allowing lithium ions to be extracted from and inserted into the material during the operation of the electrochemical system. FIG. 6 shows a cyclic voltammogram of LiFePCL electrode in a mixed solution of Li2SO4 and NaCl and a pure NaCl solution. Compared to scanning in a pure NaCl solution, the redox peaks were clearly noticed for the LFP electrode in the mixed solution.

[0127] The cyclic voltammograms shown in FIG. 7 are graphical representations of the current vs. voltage for a system being cyclically charged and discharged. Symmetric curves indicate a reversible process, where the charging and discharging behaviors mirror each other. In this case, it is the intercalation (insertion) of lithium ions into the framework of the cathode material - FP and LFP - during charging and the deintercalation (removal) of the lithium ions during discharging. The fact that these curves are symmetric over a wide range of lithium concentrations indicates that these processes are highly reversible - the lithium ions can be inserted and removed efficiently - even as the concentration of lithium ions changes. At low lithium concentrations (e.g., between 10-100 ppm), a salt (e.g., potassium chloride; KC1) is added to the system to adjust the conductivity (the ability of the solution to transmit current). Adjusting the conductivity allowed lithium to be extracted more efficiently.Table 1. Example of Conductivity of the system changes with different lithium concentrations

[0128] FIG. 8A-8D show that LFP works in various brines. Cyclic voltammetry was conducted at ImV / s and 0.1 mV / s. Among them, the LFP shows the best performance in the first (8A) and the second (8B) brines. Conductivity was larger than standard 5000 ppm Li from sulfate (around 35 mS / cm).

[0129] The performance of a LFP electrode in various brine solutions was tested, with results depicted in FIG. 8A-8D. The voltammetry was conducted at two different scan rates, 1 mV / s and 0.1 mV / s. The LFP electrode performed best in the brine solutions tested in FIG. 8A and 8B. The conductivity of these brine solutions was larger than that of a standard 5000 ppm lithium from sulfate solution (which had conductivity around 35 mS / cm). Conductivity is an important parameter in these tests because it affects the ion transport and hence, the extraction performance. Higher conductivity indicates more efficient transport of ions, which could potentially lead to improved extraction rate.

[0130] In some embodiments, the intermediate electrode comprises a metal current collector or a carbon current collector. In some embodiments, the intermediate electrode comprises a metal current collector. In some embodiments, the metal current collector comprises copper (Cu), titanium (Ti), aluminum (Al), magnesium (Mg), zinc (Zn), tin (Sn), or any metal that is capable of forming an alloy with lithium. In some embodiments, the current collector comprises vanadium oxide (V2O5). In some embodiments, the current collector comprises metal oxide. In some embodiments, the intermediate electrode comprises a carbon current collector. In some embodiments, the carbon current collector comprises graphite.

[0131] In some embodiments, the metal current collector comprises copper, aluminum, graphite- coated copper, nickel, silicon, silver, carbon (e.g., rough-surface carbon, graphene), a lithophilic material, aluminum, gold, a copper alloy (Cu-Ni, Cu-Ti, Cu-Zn, Cu-Al, Cu-Sn), or any combination thereof, the metal current collector substrate comprises Cu-Ni, Cu-Ti, Cu-Zn, Cu- Al, Cu-Sn, Ni-CO, Al-Mg, Fe-Cr-Ni, or any combination thereof. In some embodiments, the intermediate electrode comprises a lithium absorption electrode comprising graphite or metals that alloy with lithium.

[0132] In some embodiments, a current collector may have a thickness of at least 1, 2, 3, 4, 5, 6,7, 8, 9, 10, 20, 30, 40, 50, 60, 70, 80, 90, 100, 200, 300, 400, 500, 600, 700, 800, 900, or 1000 pm. In some embodiments, a current collector may have a thickness of at most 1, 2, 3, 4, 5, 6, 7,8, 9, 10, 20, 30, 40, 50, 60, 70, 80, 90, 100, 200, 300, 400, 500, 600, 700, 800, 900, or 1000 pm. In some embodiments, a current collector comprises copper, stainless steel, aluminum, nickel, titanium, sintered carbon, copper or stainless steel that is surface-treated with carbon, nickel, titanium or silver, and aluminum-cadmium alloys In some embodiments, a current collector comprises fine irregularities on surfaces thereof so as to enhance adhesive strength of the positive electrode current collector to the positive electrode active material. In some embodiments, a current collector comprises can comprise various forms including films, sheets, foils, nets, porous structures, foams, and non-woven fabrics. In some embodiments, a current collector comprises carbon, carbon paper, carbon cloth or a metal or noble metal mesh or foil.

[0133] In some embodiments, the intermediate electrode comprises an electrically conductive slurry comprising an electrically conductive additive. In some embodiments, the electrically conductive additive comprises carbon.

[0134] In some embodiments, the intermediate electrode is substantially non-reactive with nonlithium components in the aqueous source.

[0135] In some embodiments, the intermediate electrode is reactive with non-lithium components in the aqueous source. In that case, the intermediate electrode and a nonaqueous / polymer electrolyte can be physically separated from a counter (positive) electrode and the aqueous source comprising lithium by a lithium ion-selective membrane. The lithium ion-selective membrane can permit lithium ions to flow through to the intermediate electrode selectively. In some embodiments, the lithium ion-selective membrane can substantially prevent or inhibit the passage of organic solvents, anions of lithium salts, water, or a contaminant from being transferred between the intermediate electrode and the counter (positive) electrode. The membrane can prevent the passage of lithium-reactive components (e.g., non-lithium ions, or solvents) from the counter (positive) electrode side to the intermediate electrode side, to prevent or inhibit the formation of a solid electrolyte interphase. In some embodiments, the lithium ion- selective membrane comprises a single layer or multiple layers. In some embodiments, the lithium ion-selective membrane comprises glass fiber, polyester, polyethylene, polypropylene, polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), and a combination thereof. In some embodiments, the lithium ion-selective membrane comprises hydrophobic polymers. In some embodiments, the lithium ion-selective membrane comprises lithium-ion conductive channels.

[0136] In some embodiments, the intermediate electrode can be a positive electrode. In some embodiments, the intermediate electrode is a lithium-rich intermediate electrode. In some embodiments, the lithium-rich intermediate electrode comprises 10 atomic % (at%), 12 at%, 14 at%, 16 at%, 18 at%, 20 at%, 22 at%, 24 at%, 26 at%, 28 at%, 30 at%, 32 at%, 34 at%, 36 at%, 38 at%, 40 at%, 42 at%, 44 at%, 46 at%, 48 at%, 50 at%, 52 at%, 54 at%, 56 at%, 58 at%, or 60 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises about 10 at%, 12 at%, 14 at%, 16 at%, 18 at%, 20 at%, 22 at%, 24 at%, 26 at%, 28 at%, 30 at%, 32 at%, 34 at%, 36 at%, 38 at%, 40 at%, 42 at%, 44 at%, 46 at%, 48 at%, 50 at%, 52 at%, 54 at%, 56 at%, 58 at%, or 60 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 10 atomic % (at%), 12 at%, 14 at%, 16 at%, 18 at%, 20 at%, 22 at%, 24 at%, 26 at%, 28 at%, 30 at%, 32 at%, 34 at%, 36 at%, 38 at%, 40 at%, 42 at%, 44 at%, 46 at%, 48 at%, 50 at%, 52 at%, 54 at%, 56 at%, 58 at%, or 60 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 10 at%, 12 at%, 14 at%, 16 at%, 18 at%, 20 at%, 22 at%, 24 at%, 26 at%, 28 at%, 30 at%, 32 at%, 34 at%, 36 at%, 38 at%, 40 at%, 42 at%, 44 at%,46 at%, 48 at%, 50 at%, 52 at%, 54 at%, 56 at%, 58 at%, or 60 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 10 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 12 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 14 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 16 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 18 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 20 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 22 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 24 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 26 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 28 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 30 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 32 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 34 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 36 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 38 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 40 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 42 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 44 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 46 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 48 at% more than a minimum amount of-SO-lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 50 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 52 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 54 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 56 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 58 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 60 at% more than a minimum amount of lithium that can be present.

[0137] In some embodiments, the lithium-rich intermediate electrode comprises at least 10 mole%, 12 mole%, 14 mole%, 16 mole%, 18 mole%, 20 mole%, 22 mole%, 24 mole%, 26 mole%, 28 mole%, 30 mole%, 32 mole%, 34 mole%, 36 mole%, 38 mole%, 40 mole%, 42 mole%, 44 mole%, 46 mole%, 48 mole%, 50 mole%, 52 mole%, 54 mole%, 56 mole%, 58 mole%, or 60 mole% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 10 mole% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 12 mole% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 14 mole% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 16 mole% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 18 mole% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 20 mole% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 22 mole% more than a minimum amount of lithium that can be present. In some embodiments, the lithium -rich intermediate electrode comprises at least 24 mole% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 26 mole% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 28 mole% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 30 mole% more than a minimum amount of lithium that can be present. In some embodiments,the lithium-rich intermediate electrode comprises at least 32 mole% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 34 mole% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 36 mole% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 38 mole% more than a minimum amount of lithium that can be present. In some embodiments, the lithium -rich intermediate electrode comprises at least 40 mole% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 42 mole% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 44 mole% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 46 mole% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 48 mole% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 50 mole% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 52 mole% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 54 mole% more than a minimum amount of lithium that can be present. In some embodiments, the lithium -rich intermediate electrode comprises at least 56 mole% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 58 mole% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 60 mole% more than a minimum amount of lithium that can be present.

[0138] In some embodiments, the lithium-rich intermediate electrode comprises at most 10 atomic % (at%), 12 at%, 14 at%, 16 at%, 18 at%, 20 at%, 22 at%, 24 at%, 26 at%, 28 at%, 30 at%, 32 at%, 34 at%, 36 at%, 38 at%, 40 at%, 42 at%, 44 at%, 46 at%, 48 at%, 50 at%, 52 at%, 54 at%, 56 at%, 58 at%, or 60 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 10 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 12 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 14 at% of amaximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 16 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 18 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 20 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 22 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 24 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 26 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 28 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 30 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 32 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 34 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 36 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 38 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 40 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 42 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 44 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 46 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 48 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 50 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 52 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 54 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 56 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 58 at%of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 60 at% of a maximum amount of lithium that can be present.

[0139] In some embodiments, the lithium-rich intermediate electrode comprises at most 10 mole%, 12 mole%, 14 mole%, 16 mole%, 18 mole%, 20 mole%, 22 mole%, 24 mole%, 26 mole%, 28 mole%, 30 mole%, 32 mole%, 34 mole%, 36 mole%, 38 mole%, 40 mole%, 42 mole%, 44 mole%, 46 mole%, 48 mole%, 50 mole%, 52 mole%, 54 mole%, 56 mole%, 58 mole%, or 60 mole% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 10 mole% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 12 mole% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 14 mole% of a maximum amount of lithium that can be present. In some embodiments, the lithium- rich intermediate electrode comprises at most 16 mole% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 18 mole% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 20 mole% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 22 mole% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 24 mole% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 26 mole% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 28 mole% of a maximum amount of lithium that can be present. In some embodiments, the lithium- rich intermediate electrode comprises at most 30 mole% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 32 mole% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 34 mole% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 36 mole% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 38 mole% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 40 mole% of a maximum amount of lithium that can bepresent. In some embodiments, the lithium-rich intermediate electrode comprises at most 42 mole% of a maximum amount of lithium that can be present. In some embodiments, the lithium- rich intermediate electrode comprises at most 44 mole% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 46 mole% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 48 mole% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 50 mole% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 52 mole% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 54 mole% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 56 mole% of a maximum amount of lithium that can be present. In some embodiments, the lithium- rich intermediate electrode comprises at most 58 mole% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 60 mole% of a maximum amount of lithium that can be present.

[0140] For example, in the case of Li(i-X)FePO4, x ranges from 1 to 0 by fully lithiating it in the brine source, and then 0 to 1 by de-lithiating the intermediate electrode. The atomic % of lithium refers to 100*(l-x) / [(l-x) +6],

[0141] In some embodiments, the intermediate electrode can be used as a lithium source for transferring lithium to the current collector substrate. In some embodiments, the lithium-rich intermediate electrode comprises lithium iron phosphate (LiFePCU, LFP), lithium nickel manganese cobalt oxide (LiNiMnCoCh, NMC), lithium manganate (Li2MnO4, LMO), LiCe, LixMgy, LixAly, LixSiy, or a combination thereof.

[0142] In some embodiments, the lithium-rich intermediate electrode can be physically separated from a counter (negative) electrode or a current collector substrate by a lithium ion-selective membrane. The lithium ion-selective membrane can permit lithium ions to flow through to a counter (negative) electrode or a current collector substrate selectively. In some embodiments, the lithium ion-selective membrane can substantially prevent or inhibit the passage of organic solvents, anions of lithium salts, water, or a contaminant from being transferred between the lithium-rich intermediate electrode and a counter (negative) electrode or a current collector substrate. The membrane can prevent the passage of lithium-reactive components (e.g., nonlithium ions, or solvents) between the lithium-rich intermediate electrode side and a counter(negative) electrode or a current collector substrate side. In some embodiments, the lithium ion- selective membrane comprises a single layer or multiple layers. In some embodiments, the lithium ion-selective membrane comprises glass fiber, polyester, polyethylene, polypropylene, polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), and a combination thereof. In some embodiments, the lithium ion-selective membrane comprises hydrophobic polymers. In some embodiments, the lithium ion-selective membrane comprises lithium-ion conductive channels.

[0143] In some embodiments, the intermediate electrode can be in a roll form. In some embodiments, the intermediate electrode can be a coiled electrode. In some embodiments, a coiled electrode can have larger surface area than a non-coiled electrode. This increased surface area can allow for more chemical reactions to occur, which can result in a higher energy density and improved battery performance. In some embodiments, a coiled electrode can provide enhanced power output. In some embodiments, a coiled electrode can allow for better current flow within the battery than a non-coiled electrode. In some embodiments, a coiled battery can deliver power more efficiently and effectively than a non-coiled electrode. In some embodiments, a coiled electrode can improve the stability and longevity of a battery. In some embodiments, by arranging the electrodes in a coiled form, the stress and strain on the active materials within the battery can be reduced. In some embodiments, a coiled electrode can provide design flexibility. In some embodiments, by using a coiled electrode design, batteries can be more flexible, allowing for their integration into various devices like wearables or bendable electronics. This flexibility can expand the potential applications of batteries and open up new possibilities for portable and flexible devices.SEPARATOR

[0144] In some embodiments, the intermediate electrode is reactive with non-lithium components in the aqueous source. In that case, the intermediate electrode and a nonaqueous / polymer electrolyte can be physically separated from a counter (positive) electrode and the aqueous source comprising lithium by a separator. In some embodiments, the separator is placed between the intermediate electrode and the counter electrode. In some embodiments, the separator is placed between the intermediate electrode and the current collector substrate. In some embodiments, the separator can be in contact with the layer of lithium metal. In some embodiments, the separator comprises a polymer membrane or a ceramic membrane. The separator can be wetted with an electrolyte. The separator can comprise a surface that is substantially non-reactive with lithium metal. In some embodiments, the separator is a solid. Insome embodiments, the separator is configured to function as a solid state electrolyte. In some embodiments, the intermediate electrode is physically separated from the current collector substrate by a separator. In some embodiments, lithium-rich intermediate electrode can be used for transferring the lithium to a current collector substrate to form an electrode without any cleaning or drying processes.

[0145] In some embodiments, the separator can be configured to selectively conduct lithium ions, while preventing the passage of water. In some embodiments, the separator can comprise a polymer, a ceramic, or both. In some embodiments, the separator can comprise a composite comprising a polymer and a plurality of lithium ion conductive particles. In some embodiments, the separator can be configured to function as a solid state electrolyte.

[0001] In some embodiments, the separator comprises a composite membrane comprising lithium ion conductive polymers. The lithium ion conductive polymers can be flexible and moldable for various form factors, and may lack certain manufacturing challenges associated with ceramic compositions.

[0002] In some aspects, the conductive composite membranes can be configured to block the passage of water molecules from a lithium resource, such as brine, to a working electrode when electrodepositing lithium. Conductive composite membranes disclosed herein can comprise a combination of one or more lithium ion conductive particles and a polymer. In some embodiments, the lithium ion conductive particles can comprise a solid ion conductive material. In some embodiments, the polymer can comprise a hydrophobic polymer.

[0146] Without being bound to a particular theory, the composite membrane can provide boundaries between particles and the polymer that creates an interface, where lithium ions can rapidly diffuse in the interface. Using lithium ion conductive particles can further provide additional diffusivity for lithium ions through the particles and thereby the composite membrane.

[0147] In some embodiments, the polymer of the conductive composite membrane does not conduct lithium ions. In some embodiments, the polymer comprises a hydrophobic polymer. The hydrophobic polymer can comprise, e.g., a cyclic olefin copolymer, fluorinated ethylene propylene, ethylene-methyl acrylate copolymer, perfluoroalkoxy polymer, polymethylpentene, polypropylene, polyphenylene sulfide, polystyrene, polytetrafluoroethylene, polyvinylchloride, polyethylene, ethylene vinyl acetate, poly(chlorotrifluoroethylene), polyester, parylene, polycarbonate, polybutadiene or any combination thereof. In some embodiments, the polymer comprises a cyclic olefin copolymer (COC) with a heat deflection temperature of 75 °C. In some embodiments, the polymer can comprise an olefin polymer. In some embodiments, the polymercan comprise a non-olefin polymer. In some embodiments, the polymer can comprise a cyclic polymer. In some embodiments, the polymer can comprise an acrylic polymer. In some embodiments, the polymer can comprise a copolymer. In some embodiments, the polymer can comprise an amorphous domain. In some embodiments, the polymer can comprise a crystalline domain. In some embodiments, the polymer can comprise a cyclic olefin copolymer. The cyclic olefin copolymer can comprise an amorphous polymer produced by, e.g., copolymerization of cyclic monomers with ethylene. Some examples of cyclic monomers comprise 8,9,10-trinorborn- 2-ene (norbomene) and l,2,3,4,4a,5,8,8a-octahydro-l,4:5,8-dimethanonaphthalene (tetracyclododecene). In some embodiments, the cyclic olefin copolymer comprises TOPAS® Advanced Polymers’ TOPAS, or Mitsui Chemical’s APEL®. In some embodiments, hydrophobic alkyl or fluoroalkyl chains may be grafted onto the surface of the polymer matrix to increase it hydrophobicity. In some embodiments, the hydrophobic alkyl or fluoroalkyl chains grafted to the polymer matrix may enhance water blocking capability of the polymer.

[0148] In some embodiments, the conductive composite membrane can comprise low water permeability and low pore volumes. Water permeability of the conductive composite membrane can be measured by various techniques. One technique is Near-Infrared (NIR) spectroscopy. In some embodiments, a NIR measurement can report a water permeability of the conductive composite membrane of less than 1.0 nL / cm2 / min under 1 mA / cm2. In some embodiments, a NIR measurement can report a water permeability of the conductive composite membrane of less than 10, 9, 8, 7, 6, 5, 4, 3, 2, 1, 0.9, 0.8, 0.7, 0.6, 0.5, 0.4, 0.3, 0.2, or 0. nL / cm2 / min under a current density of 10, 9, 8, 7, 6, 5, 4, 3, 2, 1, 0.9, 0.8, 0.7, 0.6, 0.5, 0.4, 0.3, 0.2, or 0.1 mA / cm2. In some embodiments, a NIR measurement can report a water permeability of the conductive composite membrane as greater than 1.0 nL / cm2 / min under 1 mA / cm2. In some embodiments, a NIR measurement can report a water permeability of the conductive composite membrane as greater than 10, 9, 8, 7, 6, 5, 4, 3, 2, 1, 0.9, 0.8, 0.7, 0.6, 0.5, 0.4, 0.3, 0.2, or 0.1 nL / cm2 / min under a current density of 10, 9, 8, 7, 6, 5, 4, 3, 2, 1, 0.9, 0.8, 0.7, 0.6, 0.5, 0.4, 0.3, 0.2, or 0.1 mA / cm2. In some embodiments, the composite membrane has a water permeability of less than 10'10m2s'1Pa'1, 10'15m2s'1Pa'1, 10'18m2s'1Pa'1, or 10'21m2s'1Pa'1under 1 mA / cm2of the current density as measured at least in part by Near-Infrared (NIR) spectroscopy. In some embodiments, the composite membrane has a water permeability of less than 10'21m2s'1Pa'1under 1 mA / cm2of the current density as measured at least in part by Near-Infrared (NIR) spectroscopy. Pore volume of the conductive composite membrane can be measured by various techniques. One technique for measuring pore volume is gas pycnometry. In some embodiments,the conductive composite membrane comprises less than 30% pores by volume. In some embodiments, the conductive composite membrane comprises greater than 30% pores by volume. In some embodiments, the conductive composite membrane comprises less than 50, 40, 30, 20, 10, 9, 8, 7, 6, 5, 4, 3, 2, 1% pores by volume. In some embodiments, the conductive composite membrane comprises greater than 50, 40, 30, 20, 10, 9, 8, 7, 6, 5, 4, 3, 2, 1% pores by volume.

[0149] The conductive composite membrane can comprise various values of Li+conductivity. The conductivity can depend on various fabrication parameters, such as the choice of materials, particle density, and other parameters detailed herein. The conductivity can also depend on temperature, as the conductivity usually varies with temperature (e.g., which may be approximated by the Arrhenius relation). The conductivity of the conductive composite membrane can be increased by fabricating it with using polymers that have high decomposition temperatures, which can accordingly be used at high temperatures to conduct lithium ions. In some embodiments, the conductive composite membrane comprises a Li+conductivity of at least 10'7, 10'6, 10'5, 10'5, 10'4, 10'3, or 10'2S / cm. In some embodiments, the conductive composite membrane comprises a Li+conductivity of at most 10'7, 10'6, 10'5, 10'5, 10'4, 10'3, or 10'2S / cm. In some embodiments, the conductive composite membrane comprises a Li+conductivity of at least 1.0 x io-5S / cm. In some embodiments, the conductive composite membrane comprises a Li+conductivity of at most 1.0 x 10'5S / cm. In some embodiments, the conductive composite membrane comprises a Li+conductivity of at least 0.1, 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8, 0.9, 1, 2, 3, 4, 5, 6, 7, 8, or 9 x 10'5S / cm. In some embodiments, the conductive composite membrane comprises a Li+conductivity of at least 0.1, 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8, 0.9, 1, 2, 3, 4, 5, 6, 7, 8, or 9 x 10'4S / cm. In some embodiments, the conductive composite membrane comprises a Li+conductivity of at least 0.1, 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8, 0.9, 1, 2, 3, 4, 5, 6, 7, 8, or 9 x 10'3S / cm. In some embodiments, the conductive composite membrane comprises a Li+conductivity of at least 0.1, 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8, 0.9, 1, 2, 3, 4, 5, 6, 7, 8, or 9 x IO’2S / cm. In some embodiments, the conductive composite membrane comprises a Li+conductivity of at most 0.1, 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8, 0.9, 1, 2, 3, 4, 5, 6, 7, 8, or 9 x 10'5S / cm. In some embodiments, the conductive composite membrane comprises a Li+conductivity of at most 0.1, 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8, 0.9, 1, 2, 3, 4, 5, 6, 7, 8, or 9 x 10'4S / cm. In some embodiments, the conductive composite membrane comprises a Li+conductivity of at most 0.1, 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8, 0.9, 1, 2, 3, 4, 5, 6, 7, 8, or 9 x 10'3S / cm. In some embodiments, the conductive composite membrane comprises a Li+conductivity of at most 0.1, 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8, 0.9, 1, 2,3, 4, 5, 6, 7, 8, or 9 x 10'2S / cm. In some embodiments, the conductive composite membrane comprises a Li+conductivity from 10'4to 10'2S / cm. In some embodiments, the conductive composite membrane comprises an activation energy for lithium conductivity of about 0.2 to 0.8 eV. In some embodiments, the conductive composite membrane comprises an activation energy for lithium conductivity that is at least 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, or 0.8 eV. In some embodiments, the conductive composite membrane comprises an activation energy for lithium conductivity that is at most 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, or 0.8 eV. The activation energy can be obtained, e.g., by measuring the lithium conductivity at various temperatures and fitting the measured conductivities to the Arrhenius equation. The slope of the logarithm of conductivity as a function of the inverse temperature can lead to the activation energy.

[0150] The conductive composite membrane can comprise mechanical properties that permit scalability and application in industrial settings. In some embodiments, the conductive composite membrane can comprise a curved form factor. For example, the conductive composite membrane can be formed into various shapes, including bended shapes. The conductive composite membrane can be rolled, folded, or etc. In some embodiments, the conductive composite membrane comprises a Young’s modulus of less than 10 GPa. In some embodiments, the conductive composite membrane comprises a Young’s modulus of less than 0.1, 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8, 0.9, 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 20, 30, 40, 50, 60, 70, 80, 90, or 100 GPa. In some embodiments, the conductive composite membrane comprises a Young’s modulus of greater than 0.1, 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8, 0.9, 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 20, 30, 40, 50, 60, 70, 80, 90, or 100 GPa. In some embodiments, the conductive composite membrane is bendable to a radius of curvature of at least 1 mm without substantially affecting a water impermeability and / or the Li+conductivity of the conductive composite membrane. In some embodiments, the conductive composite membrane is bendable to a radius of curvature of at least 0.1, 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8, 0.9, 1, 2, 3, 4, 5, 6, 7, 8, 9, or 10 mm without substantially affecting a water impermeability and / or the Li+conductivity of the conductive composite membrane. In some embodiments, the conductive composite membrane is bendable to a radius of curvature of at most 0.1, 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8, 0.9, 1, 2, 3, 4, 5, 6, 7, 8, 9, or 10 mm without substantially affecting a water impermeability and / or the Li+conductivity of the conductive composite membrane.

[0151] In some embodiments, the separator comprises a lithium ion-selective membrane. The lithium ion-selective membrane can permit lithium ions to flow through to the intermediate electrode selectively. In some embodiments, the lithium ion-selective membrane cansubstantially prevent or inhibit the passage of organic solvents, anions of lithium salts, water, or a contaminant from being transferred between the intermediate electrode and the counter (positive) electrode. The membrane can prevent the passage of lithium-reactive components (e.g., non-lithium ions, or solvents) from the counter (positive) electrode side to the intermediate electrode side, to prevent or inhibit the formation of a solid electrolyte interphase. In some embodiments, the lithium ion-selective membrane can substantially prevent or inhibit the passage of organic solvents, anions of lithium salts, water, or a contaminant from being transferred between the intermediate electrode and the current collector substrate. In some embodiments, the lithium ion-selective membrane comprises a single layer or multiple layers. In some embodiments, the lithium ion-selective membrane comprises glass fiber, polyester, polyethylene, polypropylene, polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), and a combination thereof. In some embodiments, the lithium ion-selective membrane comprises hydrophobic polymers. In some embodiments, the lithium ion-selective membrane comprises lithium-ion conductive channels. In some embodiments, the lithium ion-selective membrane comprises a polymeric matrix and a plurality of ion-conducting particles disposed within the polymeric matrix. In some embodiments, the lithium ion-selective membrane comprises a glass frit with lithium ion conducting particles disposed within.

[0152] In some embodiments, the lithium ion-selective membrane comprises a polymeric matrix and a plurality of ion-conducting particles disposed within the polymeric matrix.

[0153] In some embodiments, the lithium ion-selective membrane is a hybrid organic-inorganic membrane including a polymeric matrix and a plurality of ion-conducting particles disposed within the polymeric matrix. In some such embodiments, an inorganic coating is deposited on the polymeric matrix, the inorganic coating being a uniform layer of 1 to 10,000 atoms thick. In some embodiments, the polymer can be a silica-based polyurethane, polyethylene oxide, polystyrene, or polyamide. In some embodiments, the lithium ion-selective membrane comprises a glass frit with lithium ion conducting particles disposed within.

[0154] In some embodiments, the ion conducting particles are selected from the group consisting of LiFePC , LiCoCCh, NASICON (sodium superionic conductor, Na3Zr2Si2POi2) electrolytes, lithium-lanthanum titanates (LLTO), garnet type electrolytes, LISICON (Lithium Super Ionic CONductor, Li2+2xZ xGeCU) and Thio-LISICON electrolytes, LiyLasZ^On (LLZO, lithium lanthanum zirconium oxide), the cubic phase (c-LLZO).

[0155] In some embodiments, the polymer membrane can comprise a hydrophilic polymer. In some embodiments, the polymer membrane can comprise a hydrophobic polymer. In someembodiments, the polymer can be glassy at room temperature. In some embodiments, the polymer can be a melt at room temperature. In some embodiments, the polymer membrane can selectively conduct and / or diffuse lithium ions over magnesium ions, calcium ions, sodium ions, or any combination thereof. In some embodiments, the polymer membrane can comprise a lithium ion to magnesium ion selectivity of at least 10, 50, 100, 500, 1000, 5000, or 10000. In some embodiments, the polymer membrane can comprise a lithium ion to magnesium ion selectivity of at most 10, 50, 100, 500, 1000, 5000, or 10000. In some embodiments, the polymer membrane can comprise a lithium ion to sodium ion selectivity of at least 10, 50, 100, 500, 1000, 5000, or 10000. In some embodiments, the polymer membrane can comprise a lithium ion to sodium ion selectivity of at most 10, 50, 100, 500, 1000, 5000, or 10000. In some embodiments, the polymer membrane can comprise a lithium ion to calcium ion selectivity of at least 10, 50, 100, 500, 1000, 5000, or 10000. In some embodiments, the polymer membrane can comprise a lithium ion to calcium ion selectivity of at most 10, 50, 100, 500, 1000, 5000, or 10000. For example, the polymer can comprise cellulose. In some embodiments, the polymer can comprise cellulose diacetate, cellulose triacetate, cellulose nitrate, cellulose acetate butyrate, or a combination thereof. The cellulose can be at least 5, 10, 20, 30, 40, 50, 60, 70, or 80 percent acetylated. The cellulose can be at most 5, 10, 20, 30, 40, 50, 60, 70, or 80 percent acetylated.

[0156] In some embodiments, the polymer membrane comprises anisotropic properties. In some embodiments, the polymer membrane comprises a lithium conductivity that is different in the direction perpendicular to the plane of the polymer membrane, compared to the direction that is parallel to the plane of the polymer membrane. For example, when the polymer membrane is spin cast or extruded, the properties of the polymer membrane may be different in the planar direction when the molecules of the polymer become partially aligned due to shear forces. In some embodiments, the polymer membrane can become isotropic when the polymer molecules are given sufficient time to relax and reorganize to an isotropic state.

[0157] In some embodiments, the polymer membrane comprises pores. In some embodiments, the polymer membrane can comprise manufacturing defects which can sporadically introduce air bubbles which occupy a certain amount of space in the polymer. In some embodiments, the polymer membrane can be nonporous when the air bubbles are sufficiently annealed out of the polymer membrane.

[0158] In some embodiments, the polymer membrane is semi-crystalline. In some embodiments, the polymer membrane comprises a crystallinity of at least 0, 5, 10, 15, or 20 percent. In someembodiments, the polymer membrane comprises a crystallinity of at most 0, 5, 10, 15, or 20 percent.

[0159] In some embodiments, the polymer membrane can comprise a thickness of at least 0.1, 0.5, 1, 5, 10, 50, 100, 200, 300, 400, or 500 microns. In some embodiments, the polymer membrane can comprise a thickness of at most 0.1, 0.5, 1, 5, 10, 50, 100, 200, 300, 400, or 500 microns. In some embodiments, the polymer membrane comprises a glass transition temperature of at least 25, 50, 75, 100, 250, 450, or 500 °C. In some embodiments, the polymer membrane comprises a glass transition temperature of at most 25, 50, 75, 100, 250, 450, or 500 °C.

[0160] In some embodiments, the polymer membrane is a monovalent selective ion exchange membrane. In some embodiments, electrodialysis can be performed to a lithium resource using a polymer membrane to extract lithium from the lithium resource. In some embodiments, the monovalent selective cation exchange membrane comprises a modified surface. In some embodiments, the modified surface comprises charge moieties to provide a larger Coulombic energy barrier against some ions than other ions. In some embodiments, the membrane is an anion exchange membrane. In some embodiments, the charge moiety can be an amine or an ammonium group. In some embodiments, the anion exchange membrane is configured to selectively extract monovalent anions, such as chlorine or bromine ions, over multivalent anions, such as sulfate ions.

[0161] In some embodiments, an alkyl of the ammonium group of the membrane can be varied to provide different degrees of hydrophobicity. In some embodiments, the ammonium group can be a primary ammonium, a secondary ammonium, a tertiary ammonium, or a quaternary ammonium group. The alkyl group can be a methyl, ethyl, propyl, butyl, pentyl, hectyl, heptyl, octyl, nonyl, decyl, undecyl, dodecyl, or a longer alkyl group.

[0162] In some embodiments, the membrane comprises a water content of at least 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 15, 20, 25, 30, 35, or 40 percent by weight in operation. In some embodiments, the membrane comprises a water content of at most 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 15, 20, 25, 30, 35, or 40 percent by weight in operation. In some embodiments, the membrane comprises a resistivity of at least 0.5, 1, 1.5, 2, 2.5, 3, 3.5, 4, 4.5, 5, 5.5, or 6 Q-cm2. In some embodiments, the membrane comprises a resistivity of at most 0.5, 1, 1.5, 2, 2.5, 3, 3.5, 4, 4.5, 5, 5.5, or 6 -cmA2. In some embodiments, the membrane comprises a Donnan potential of at least 1, 2, 3, 4, 5, 10, 15, 20, 25, or 30 mV in operation. In some embodiments, the membrane comprises a Donnan potential of at most 1, 2, 3, 4, 5, 10, 15, 20, 25, or 30 mV in operation. In some embodiments, the membrane can be used with a current density of at least 100, 200, 300, 400, 500, 1000, or 2000A / m2. In some embodiments, the membrane can be used with a current density of at most 100, 200, 300, 400, 500, 1000, or 2000 A / m2.

[0163] In some embodiments, the membrane is configured to block the transport of protons. In some embodiments, the membrane does not comprise a percolating network of water molecules. In some embodiments, the membrane have an aprotic chemistry. In some embodiments, the membrane comprises polar functional groups capable of conducting lithium ions.

[0164] In some embodiments, the separator comprises a porosity of 10 percent (%), 20 %, 30 %, 40 %, 50 %, 60 %, 70 %, or 80 %. In some embodiments, the separator comprises a porosity of about 10 %, about 20 %, about 30 %, about 40 %, about 50 %, about 60 %, about 70 %, or about 80 %. In some embodiments, the separator comprises a porosity of at least 10 %, at least 20 %, at least 30 %, at least 40 %, at least 50 %, at least 60 %, at least 70 %, or at least 80 %. In some embodiments, the separator comprises a porosity of at most 10 %, at most 20 %, at most 30 %, at most 40 %, at most 50 %, at most 60 %, at most 70 %, or at most 80 %. The separator can have a porosity of at least 55%. The separator can have a porosity of at most 55%. The separator can have a porosity of about 55%.

[0165] In some embodiments, a thickness of the separator is 5 pm, 10 pm, 15 pm, 20 pm, 25 pm, 30 pm, 35 pm, 40 pm, 45 pm, 50 pm, 60 pm, 70 pm, 80 pm, 90 pm, 100 pm, 120 pm, 140 pm, 160 pm, 180 pm, 200 pm, 300 pm, 400 pm, or 500 pm. In some embodiments, a thickness of the separator is about 5 pm, about 10 pm, about 15 pm, about 20 pm, about 25 pm, about 30 pm, about 35 pm, about 40 pm, about 45 pm, about 50 pm, about 60 pm, about 70 pm, about 80 pm, about 90 pm, about 100 pm, about 120 pm, about 140 pm, about 160 pm, about 180 pm, about 200 pm, about 300 pm, about 400 pm, or about 500 pm. In some embodiments, a thickness of the separator is at least 5 pm, at least 10 pm, at least 15 pm, at least 20 pm, at least 25 pm, at least 30 pm, at least 35 pm, at least 40 pm, at least 45 pm, at least 50 pm, at least 60 pm, at least 70 pm, at least 80 pm, at least 90 pm, at least 100 pm, at least 120 pm, at least 140 pm, at least 160 pm, at least 180 pm, at least 200 pm, at least 300 pm, at least 400 pm, or at least 500 pm. In some embodiments, a thickness of the separator is at most 5 pm, at most 10 pm, at most 15 pm, at most 20 pm, at most 25 pm, at most 30 pm, at most 35 pm, at most 40 pm, at most 45 pm, at most 50 pm, at most 60 pm, at most 70 pm, at most 80 pm, at most 90 pm, at most 100 pm, at most 120 pm, at most 140 pm, at most 160 pm, at most 180 pm, at most 200 pm, at most 300 pm, at most 400 pm, or at most 500 pm. In some embodiments, the separator can be 5 to 50 pm thick.

[0166] In some embodiments, the separator can have a machine-direction tensile strength of 40 kg / cm2, 60 kg / cm2, 80 kg / cm2, 100 kg / cm2, 120 kg / cm2, 140 kg / cm2, 160 kg / cm2, 180 kg / cm2, or 200 kg / cm2. In some embodiments, the separator can have a machine-direction tensile strength of about 40 kg / cm2, about 60 kg / cm2, about 80 kg / cm2, about 100 kg / cm2, about 120 kg / cm2, about 140 kg / cm2, about 160 kg / cm2, about 180 kg / cm2, or about 200 kg / cm2. In some embodiments, the separator can have a machine-direction tensile strength of at least 40 kg / cm2, at least 60 kg / cm2, at least 80 kg / cm2, at least 100 kg / cm2, at least 120 kg / cm2, at least 140 kg / cm2, at least 160 kg / cm2, at least 180 kg / cm2, or at least 200 kg / cm2. In some embodiments, the separator can have a machine-direction tensile strength of at most 40 kg / cm2, at most 60 kg / cm2, at most 80 kg / cm2, at most 100 kg / cm2, at most 120 kg / cm2, at most 140 kg / cm2, at most 160 kg / cm2, at most 180 kg / cm2, or at most 200 kg / cm2.

[0167] In some embodiments, the separator can have a transverse -direction tensile strength of 40 kg / cm2, 60 kg / cm2, 80 kg / cm2, 100 kg / cm2, 120 kg / cm2, 140 kg / cm2, 160 kg / cm2, 180 kg / cm2, or 200 kg / cm2. In some embodiments, the separator can have a transverse -direction tensile strength of about 40 kg / cm2, about 60 kg / cm2, about 80 kg / cm2, about 100 kg / cm2, about 120 kg / cm2, about 140 kg / cm2, about 160 kg / cm2, about 180 kg / cm2, or about 200 kg / cm2. In some embodiments, the separator can have a transverse -direction tensile strength of at least 40 kg / cm2, at least 60 kg / cm2, at least 80 kg / cm2, at least 100 kg / cm2, at least 120 kg / cm2, at least 140 kg / cm2, at least 160 kg / cm2, at least 180 kg / cm2, or at least 200 kg / cm2. In some embodiments, the separator can have a transverse -direction tensile strength of at most 40 kg / cm2, at most 60 kg / cm2, at most 80 kg / cm2, at most 100 kg / cm2, at most 120 kg / cm2, at most 140 kg / cm2, at most 160 kg / cm2, at most 180 kg / cm2, or at most 200 kg / cm2.

[0168] In some embodiments, the separator can have a puncture strength of 100 gf, 150 gf, 200 gf, 250 gf, 300 gf, 350 gf, 400 gf, 450 gf, or 500 gf. In some embodiments, the separator can have a puncture strength of about 100 gf, about 150 gf, about 200 gf, about 250 gf, about 300 gf, about 350 gf, about 400 gf, about 450 gf, or about 500 gf. In some embodiments, the separator can have a puncture strength of at least 100 gf, at least 150 gf, at least 200 gf, at least 250 gf, at least 300 gf, at least 350 gf, at least 400 gf, at least 450 gf, or at least 500 gf. In some embodiments, the separator can have a puncture strength of at most 100 gf, at most 150 gf, at most 200 gf, at most 250 gf, at most 300 gf, at most 350 gf, at most 400 gf, at most 450 gf, or at most 500 gf. The separator can have a puncture strength of 200-325 gf.

[0169] In some embodiments, the separator can have a Young’s modulus of 50 MPa, 100 MPa, 150 MPa, 200 MPa, 250 MPa, 300 MPa, or 400 MPa. In some embodiments, the separator canhave a Young’s modulus of about 50 MPa, about 100 MPa, about 150 MPa, about 200 MPa, about 250 MPa, about 300 MPa, or about 400 MPa. In some embodiments, the separator can have a Young’s modulus of at least 50 MPa, at least 100 MPa, at least 150 MPa, at least 200 MPa, at least 250 MPa, at least 300 MPa, or at least 400 MPa. In some embodiments, the separator can have a Young’s modulus of at most 50 MPa, at most 100 MPa, at most 150 MPa, at most 200 MPa, at most 250 MPa, at most 300 MPa, or at most 400 MPa. The separator can have a Young’s modulus of at least 200 MPa.ELECTROLYTE

[0170] In some embodiments, the electrolyte is an aqueous electrolyte. In some embodiments, the electrolyte is brine. In some embodiments, the electrolyte is a non-aqueous electrolyte. In some embodiments, the electrolyte is a polymer electrolyte. In some embodiments, the electrolyte is an organic electrolyte. In some embodiments, the electrolyte comprises a lithium salt. In some embodiments, the electrolyte comprises an ionic liquid. In some embodiments, the electrolyte comprises a deep eutectic solvent.

[0171] In some embodiments, an electrolyte comprises a decomposition potential window of at least 2, 3, 4, 5, or 6 V. In some embodiments, an electrolyte comprises a decomposition potential window of at most 2, 3, 4, 5, or 6 V. In some embodiments, an electrolyte comprises a dielectric constant of at least 2, 5, 10, 20, 30, 40, 50, 60, 70, or 80. In some embodiments, an electrolyte comprises a dielectric constant of at most 3, 5, 10, 20, 30, 40, 50, 60, 70, 80, or 90. An electrolyte can comprise various viscosities. Polymeric or polymer solution electrolytes can comprise a large viscosity, as the viscosity can scale exponentially with the molecular weight of the polymer above a critical molecular weight (e.g., entanglement molecular weight). In some embodiments, an electrolyte comprises a viscosity of at least 0.1, 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8, 0.9, 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 20, 30, 40, 50, 60, 70, 80, 90, 100, 200, 300, 400, 500, 600, 700, 800, or 900 mPa»s. In some embodiments, an electrolyte comprises a viscosity of at least 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 20, 30, 40, 50, 60, 70, 80, 90, 100, 200, 300, 400, 500, 600, 700, 800, or 900 Pa»s. In some embodiments, an electrolyte comprises a viscosity of at least 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 20, 30, 40, 50, 60, 70, 80, 90, 100, 200, 300, 400, 500, 600, 700, 800, or 900 kPa«s. In some embodiments, an electrolyte comprises a viscosity of at most 0.1, 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8, 0.9, 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 20, 30, 40, 50, 60, 70, 80, 90, 100, 200, 300, 400, 500, 600, 700, 800, or 900 mPa»s. In some embodiments, an electrolyte comprises a viscosity of at most 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 20, 30, 40, 50, 60, 70, 80, 90, 100, 200, 300, 400, 500, 600, 700, 800, or 900Pa»s. In some embodiments, an electrolyte comprises a viscosity of at most 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 20, 30, 40, 50, 60, 70, 80, 90, 100, 200, 300, 400, 500, 600, 700, 800, or 900 kPa«s.

[0172] In some embodiments, the electrolyte comprises organic electrolytes. In some embodiments, the organic electrolyte comprises dimethyl carbonate, ethylmethyl carbonate, diethyl carbonate, ethylene carbonate, propylene carbonate, l,3-dioxolan-2-one, 4-methyl-l,3- dioxolan-2-one, oxolan-2-one, and any combination thereof. In some embodiments, the electrolyte comprises an organic carbonate compound, an ester compound, an ether compound, a ketone compound, an alcohol compound, an aprotic bipolar solvent, or a combination thereof. In some embodiments, the carbonate compound can be an open chain carbonate compound, a cyclic carbonate compound, a fluorocarbonate derivative thereof, or a combination thereof.

[0173] In some embodiments, the chain carbonate compound comprises diethyl carbonate (DEC), dimethyl carbonate (DMC), dipropyl carbonate (DPC), methylpropyl carbonate (MPC), ethylpropylcarbonate (EPC), methylethyl carbonate (MEC), and a combination thereof. In some embodiments, the cyclic carbonate compound comprises ethylene carbonate (EC), propylenecarbonate (PC), butylene carbonate (BC), fluoroethylene carbonate (FEC), vinylethylene carbonate (VEC), and a combination thereof. In some embodiments, the fluorocarbonate compound comprises fluoroethylene carbonate (FEC), 4,5-difluoroethylene carbonate, 4,4-difluoroethylene carbonate, 4,4,5-trifluoroethylene carbonate, 4, 4,5,5- tetrafluoroethylene carbonate, 4-fluoro-5-methylethylene carbonate, 4-fluoro-4-methylethylene carbonate, 4,5-difluoro-4-methylethylene carbonate, 4,4,5-trifluoro-5-methylethylene carbonate, trifluoromethylethylene carbonate, and a combination thereof. In some embodiments, the carbonate compound comprises a combination of cyclic carbonate and chain carbonate, in consideration of dielectric constant and viscosity of the electrolyte. In some embodiments, the carbonate compound comprises a mixture of such chain carbonate and / or cyclic carbonate compounds as described above with a fluorocarbonate compound. In some embodiments, the fluorocarbonate compound can increase solubility of a lithium salt to improve ionic conductivity of the electrolyte, and can facilitate formation of the thin film on the negative electrode. In some embodiments, the ester compound comprises methyl acetate, ethyl acetate, n-propyl acetate, dimethyl acetate, methyl propionate (MP), ethyl propionate, y-butyrolactone, decanolide, valerolactone, mevalonolactone, caprolactone, and methyl formate. In some embodiments, the ether compound is dibutyl ether, tetraglyme, diglyme, 1,2-dimethoxy ethane, 1,2-di ethoxy ethane, ethoxymethoxyethane, 2-methyltetrahydrofuran, and tetrahydrofuran. An example of the ketone compound is cyclohexanone. In some embodiments, the alcohol compound comprises ethylalcohol or isopropyl alcohol. In some embodiments, the aprotic solvent comprises a nitrile (such as R — CN, wherein R is a C2-C20 linear, branched, or cyclic hydrocarbon-based moiety that can include a double-bond, an aromatic ring or an ether bond), amides (such as formamide and dimethylformamide), dioxolanes (such as 1,2-dioxolane and 1,3 -di oxolane), methylsulfoxide, sulfolanes (such as sulfolane and methylsulfolane), l,3-dimethyl-2-imidazolidinone, N-methyl- 2-pyrrolidinone, nitromethane, trimethyl phosphate, triethyl phosphate, trioctyl phosphate, and triester phosphate. In some embodiments, the electrolyte comprises an aromatic hydrocarbon organic solvent in a carbonate solvent. In some embodiments, the aromatic hydrocarbon organic solvent comprises benzene, fluorobenzene, 1,2-difluorobenzene, 1,3-difluorobenzene, 1,4- difluorobenzene, 1,2,3-trifluorobenzene, 1,2,4-trifluorobenzene, chlorobenzene, 1,2- dichlorobenzene, 1,3-dichlorobenzene, 1,4-di chlorobenzene, 1,2, 3 -tri chlorobenzene, 1,2,4- trichlorobenzene, iodobenzene, 1,2-diiodobenzene, 1,3-diiodobenzene, 1,4-diiodobenzene, 1,2,3- triiodobenzene, 1,2,4-triiodobenzene, 2-fluorotoluene, 3-fluorotoluene, 4-fluorotoluene, 2,3- difluorotoluene, 2,4-difluorotoluene, 2, 5 -difluorotoluene, 2,6-difluorotoluene, 3,4- difluorotoluene, 3,5-difluorotoluene, 2,3,4-trifluorotoluene, 2,3,5-trifluorotoluene, 2,3,6- trifluorotoluene, 3,4,5-trifluorotoluene, 2,4,5-trifluorotoluene, 2,4,6-trifluorotoluene, 2- chlorotoluene, 3 -chlorotoluene, 4-chlorotoluene, 2,3-dichlorotoluene, 2,4-dichlorotoluene, 2,5- dichlorotoluene, 2,6-dichlorotoluene, 2, 3, 4-tri chlorotoluene, 2,3,5-trichlorotoluene, 2,3,6- tri chlorotoluene, 3,4,5-trichlorotoluene, 2,4,5-trichlorotoluene, 2,4,6-trichlorotoluene, 2- iodotoluene, 3 -iodotoluene, 4-iodotoluene, 2, 3 -diiodotoluene, 2,4-diiodotoluene, 2,5- diiodotoluene, 2,6-diiodotoluene, 3,4-diiodotoluene, 3,5-diiodotoluene, 2,3,4-triiodotoluene, 2,3,5-triiodotoluene, 2,3,6-triiodotoluene, 3,4,5-triiodotoluene, 2,4,5-triiodotoluene, 2,4,6- triiodotoluene, o-xylene, m-xylene, p-xylene, and combinations thereof.

[0174] In some embodiments, the electrolyte comprises polymeric electrolytes. In some embodiments, the polymer electrolyte comprises polyethylene oxide), poly(vinyl alcohol), poly(methyl methacrylate), poly(caprolactone), poly(chitosan), poly(vinyl pyrrolidone), poly(vinyl chloride), poly(vinyl fluoride), poly(imide), or any combination thereof, which can inherently conduct lithium ions or be doped with one or more lithium salts to make the polymer be lithium conductive.

[0175] In some embodiments, the electrolyte comprises ionic liquids. Any one of the ionic liquids listed on the Ionic Liquids Database (ILThermo) of the National Institute of Standards and Technology can be used.

[0176] Various lithium salts can be used. A lithium salt can comprise lithium 12- hydroxystearate, lithium acetate, lithium amide, lithium aspartate, lithium azide, lithium bis(trifluoromethanesulfonyl)imide, lithium borohydride, lithium bromide, lithium carbonate, lithium chlorate, lithium chloride, lithium citrate, lithium cyanide, lithium diphenylphosphide, lithium hexafluorogermanate, lithium hexafluorophosphate, lithium hypochlorite, lithium hypofluorite, lithium metaborate, lithium methoxide, lithium naphthalene, lithium niobate, lithium nitrate, lithium nitrite, lithium oxalate, lithium perchlorate, lithium stearate, lithium succinate, lithium sulfate, lithium sulfide, lithium superoxide, lithium tantalate, lithium tetrachloroaluminate, lithium tetrafluoroborate, lithium tetrakis(pentafluorophenyl)borate, lithium triflate, lithium tungstate, or any combination thereof. In some embodiments, an electrolyte can comprise lithium salts comprising an organic anion selected from the group consisting of trifluoromethanesulfonyl-imide (TFSI), N- butyl-N-methylpyrrolidinium bis(trifluoromethanesulfonyl)imide (PyruTFSI), trifluoromethanesulfonyl-imide, bis(trifluoromethanesulfonyl)imide (LiTFSI), l-ethyl-3 - methylimidazolium- bis(trifluoromethylsulfonyl)imide (EMI-TFSI), or any combination thereof. In some embodiments, the catholyte 290 comprises ionic liquid-forming salts dissolved in 1,3-dioxolane (DOL), 1,2 dimethoxy ethane (DME), or tetraethyl ene glycol dimethyl ether (TEGDME). In some embodiments, an electrolyte can comprise Li2SO4, Li2CO3, LiPFe, LiBF4, LiBEL, LiBO, LiDFOB, LiCICU, LiTFSI, or any combination thereof. In some embodiments, an electrolyte can comprise LiPFe, LiBF4, LiBEL, LiBO, LiDFOB, LiSbFe, LiAsFe, LiSbFe, LiCFsSOs, Li(CF3SO2)3C, Li(CF3SO2)2N, LiC4F9SO3, LiC104, LiA104, LiAICU, LiAlF4, LiBPh4, LiBioCho, CH3SO3Li, C4F3SO3Li, (CF3SO2)2NLi, LiN(CxF2x+iSO2)(CxF2y+iSO2) (wherein x and y are natural numbers), CF3CO2Li, LiCl, LiBr, Lil, LIBOB (lithium bisoxalato borate), lower aliphatic carboxylic acid lithium, lithium terphenylborate, lithium imide, or any combination thereof. In some embodiments, a concentration of the lithium salt may be in a range of about 0.1 molar (“M”) to about 2.0 M. In some embodiments, a concentration of the lithium salt is at least 0.01, 0.02, 0.03, 0.04, 0.05, 0.06, 0.07, 0.08, 0.09, 0.1, 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8, 0.9, 1.0, 1.5, 2.0, 2.5, or 3 M. In some embodiments, a concentration of the lithium salt is at most 0.01, 0.02, 0.03, 0.04, 0.05, 0.06, 0.07, 0.08, 0.09, 0.1, 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8, 0.9, 1.0, 1.5, 2.0, 2.5, or 3 M.

[0177] The electrolyte can comprise a lithium conductive polymer. The lithium conductive polymer can be a copolymer. In some embodiments, the polymer can comprise a block copolymer or a random copolymer. In some embodiments, a portion of the block copolymer is incontact with lithium metal, wherein the portion is substantially unreactive with the lithium metal. A block copolymer can, for example, be annealed to undergo microphase separation, providing an exposed hydrophobic surface that is substantially unreactive with lithium metal. Meanwhile, the block copolymer can further comprise a percolating hydrophilic domain that provides paths for lithium ions to traverse through from one side of the block copolymer to the other. In some embodiments, the block copolymer comprises diblock copolymer, triblock copolymer, triblock terpolymer, multiblock copolymer, grafted copolymer, or any combination thereof. In some embodiments, the block copolymer can comprise PDMS-PEG (e.g., poly(polydimethylsiloxane methacrylate)-b-poly(poly(ethylene glycol) methacrylate)). In some embodiments, the block copolymer can comprise POEM-b-PLMA, POEM-P(PDMSMA), PBA-b-PPEGMA, or any combination thereof. In some embodiments, a copolymer can comprise poly(butyl acrylate) (PBA), Poly(butyl methacrylate) (PBMA), Poly(lauryl methacrylate) (PLMA), Poly(ethylene) (PE), Poly(ethylene-alt-propylene) (PEP), Poly(urethane) (PU), Poly(butadiene) (PB), Poly(polyvinylidene methacrylate) (PPVDFMA), Poly (polytetrafluoroethylene methacrylate) (PPTFEMA), Poly(perfluoropolyether) (PFPE), Poly(perfluoropolyether methacrylate) (PFPEMA), Poly(perfluoropolyether acrylate) (PFPEA), Poly(poly(ethylene glycol) methacrylate) (PPEGMA), Poly(poly(ethylene glycol) acrylate) (PPEGA), Poly(perfluoropolyether methacrylate) (PFPEMA), Poly(perfluoropolyether acrylate) (PFPEA), or any combination thereof.

[0178] The hydrophobic polymer can comprise, e.g., a cyclic olefin copolymer, fluorinated ethylene propylene, ethylene-methyl acrylate copolymer, polymonochlorotrifluoroethylene, perfluoroalkoxy polymer, polymethylpentene, polypropylene, polyphenylene sulfide, polystyrene, polytetrafluoroethylene, polyvinylchloride, polyethylene, ethylene vinyl acetate, or any combination thereof.

[0179] In some embodiments, an electrolyte may be a high conductivity electrolyte with a lithium transference number > 0.3, a low flammability, and weakly solvating ability to minimize the charge transfer resistance. In some embodiments, fluorinated compounds tend to make an inorganic rich SEI layer that promotes higher coulombic efficiencies.

[0180] In some embodiments, an electrolyte may be configured to form a passivation layer upon contact with a negative electrode, a positive electrode or both. The passivation layer can be a solid. The passivation layer can be stable such that further growth of the passivation layer is limited. The passivation layer can be configured to provide a low charge-transfer impedance. In some embodiments, an electrolyte can be configured to form a passivation layer upon contactwith aluminum. In some embodiments, an electrolyte can be configured to form a passivation layer comprising AIF3. In some embodiments, an electrolyte can be stable when contacted with water. In some embodiments, an electrolyte does not produce HF when contacted with water.

[0181] In some embodiments, an electrolyte may be configured to have a 1stcycle Coulombic efficiency of at least 90, 91 92, 93, 94, 95, 96, 97, 98, 99, 99.1, 99.2, 99.3, 99.4, 99.5, 99.6, 99.7, 99.8, 99.9, 99.91, 99.92, 99.93, 99.94, 99.95, 99.96, 99.97, 99.98, or 99.99 percent when incorporated into a rechargeable energy source system of the present disclosure. In some embodiments, an electrolyte may be configured to have a 1stcycle Coulombic efficiency of at most 90, 91 92, 93, 94, 95, 96, 97, 98, 99, 99.1, 99.2, 99.3, 99.4, 99.5, 99.6, 99.7, 99.8, 99.9, 99.91, 99.92, 99.93, 99.94, 99.95, 99.96, 99.97, 99.98, or 99.99 percent when incorporated into a rechargeable energy source system of the present disclosure. FIG. 17 shows the 1stcycle Coulombic efficiency of various electrolytes.

[0182] In some embodiments, an electrolyte may be compatible with a negative electrode of the present disclosure, a positive electrode of the present disclosure, or both. In some embodiments, the electrolyte comprises a carbonate. In some embodiments, the electrolyte comprises an ether. In some embodiments, the electrolyte comprises an inorganic salt. In some embodiments, the electrolyte comprises a co-salt in addition to the inorganic salt. In some embodiments, the electrolyte comprises a solvent. In some embodiments, the electrolyte is a mixture of various electrolyte components disclosed herein. The various electrolyte components can have a wide variety of concentrations. For example, the electrolyte can comprise LP30 (1.0 M LiPF6 EC / DMC). In some embodiments, the inorganic salt can comprise LiPFe, LiDFOB, LiBOB, LiFSI, LiTFSI, LiCFsSCE, or any combination thereof. In some embodiments, the solvent can comprise EC, DMC, EMC (ethyl methyl carbonate), DOL, DME, TTE, or any combination thereof. In some embodiments, the electrolyte can comprise an additive. In some embodiments, the additive can comprise PC, FEC (fluoroethylene carbonate), VC (vinylene carbonate), LiNCE, CsNCE, or any combination thereof.METHODS

[0183] In certain aspects, this disclosure provides a method of preparing an electrode for a rechargeable energy device. In some embodiments, the method comprises (i) contacting an aqueous source comprising lithium with an intermediate electrode; (ii) extracting and transferring the lithium from the aqueous source to the intermediate electrode to form a lithium- rich intermediate electrode; and (iii) transferring the lithium from the lithium-rich intermediate electrode to a current collector substrate to form an electrode for a rechargeable energy device.In some embodiments, a process of (ii) comprises extracting the lithium from the aqueous source and transferring the lithium to the intermediate electrode to form a lithium-rich intermediate electrode.

[0184] In some embodiments, the aqueous source comprising lithium is brine. In some embodiments, the aqueous source comprising lithium further comprises Na+, K+, Mg2+, Ca2+, B(OH)4, Fe2+, Fe3+, Mn2+, MnO , MnO4, Cl’, SO42’, NH3, NH4+, NH4OH, NO2, HNO2, NO3’, an alkali metal ions, an alkali earth metal ions, or any combination thereof. In some embodiments, the aqueous source comprising lithium comprises a geological resource. In some embodiments, the aqueous source comprising lithium can be pretreated to remove Na+, K+, Mg2+, Ca2+, B(OH)4, Fe2+, Fe3+, Mn2+, MnO42, MnO4, CF, SO42’, NH3, NH4+, NH4OH, NO2, HNO2, NO3‘, an alkali metal ions, an alkali earth metal ions, or any combination thereof.

[0185] In some embodiments, a process of (ii) can be performed by connecting a counter electrode to the intermediate electrode in a circuit, using the aqueous source comprising lithium as an electrolyte. In some embodiments, the counter electrode comprises graphite, platinum (Pt), titanium (Ti), or a combination thereof. In some embodiments, the process of (ii) can be performed using an applied potential of at least 3 V, 4V, 5V, 6V, 7V, 8V, 9V, 10V, 1 IV, or 12V. In some embodiments, the process of (ii) can be performed using an applied potential of at most 3V, 4VV, 6V, 7V, 8V, 9V, 10V, 1 IV, or 12V. In some embodiments, the process of (ii) can be performed using an applied potential of about 3 V to 12V, 4V to 9V, 5V to 8V, or 6V to 7V.

[0186] In some embodiments, transferring the lithium from the aqueous source to the intermediate electrode in (ii) comprises intercalating the lithium in the intermediate electrode to form the lithium-rich intermediate electrode.

[0187] In some embodiments, an amount of the lithium transferred from the aqueous source to the intermediate electrode comprises at least 0.1 mg / hr, 0.5 mg / hr, 1 mg / hr, 5 mg / hr, 10 mg / hr, 50 mg / hr, 100 mg / hr, 150 mg / hr, 200 mg / hr, 250 mg / hr, 300 mg / hr, 350 mg / hr, 400 mg / hr, 450 mg / hr, 500 mg / hr, 550 mg / hr, 600 mg / hr, 650 mg / hr, 700 mg / hr, 750 mg / hr, 800 mg / hr, 850 mg / hr, 900 mg / hr, 950 mg / hr, 1,000 mg / hr, 1,200 mg / hr, 1,400 mg / hr, 1,600 mg / hr, 1,800 mg / hr, 2,000 mg / hr, 2,500 mg / hr, 3,000 mg / hr, 3,500 mg / hr, 4,000 mg / hr, 4,500 mg / hr, 5,000 mg / hr, 5,500 mg / hr, 6,000 mg / hr, 6,500 mg / hr, 7,000 mg / hr, 7,500 mg / hr, 8,000 mg / hr, 8,500 mg / hr, 9,000 mg / hr, 9,500 mg / hr, 10,000 mg / hr, 20,000 mg / hr, 30,000 mg / hr, 40,000 mg / hr, 50,000 mg / hr, 60,000 mg / hr, 70,000 mg / hr, 80,000 mg / hr, 90,000 mg / hr, 100,000 mg / hr, 110,000 mg / hr, or 120,000 mg / hr. In some embodiments, an amount of the lithium transferred from the aqueous source to the intermediate electrode comprises at most 0.1 mg / hr, 0.5 mg / hr, 1 mg / hr, 5 mg / hr,10 mg / hr, 50 mg / hr, 100 mg / hr, 150 mg / hr, 200 mg / hr, 250 mg / hr, 300 mg / hr, 350 mg / hr, 400 mg / hr, 450 mg / hr, 500 mg / hr, 550 mg / hr, 600 mg / hr, 650 mg / hr, 700 mg / hr, 750 mg / hr, 800 mg / hr, 850 mg / hr, 900 mg / hr, 950 mg / hr, 1,000 mg / hr, 1,200 mg / hr, 1,400 mg / hr, 1,600 mg / hr, 1,800 mg / hr, 2,000 mg / hr, 2,500 mg / hr, 3,000 mg / hr, 3,500 mg / hr, 4,000 mg / hr, 4,500 mg / hr, 5,000 mg / hr, 5,500 mg / hr, 6,000 mg / hr, 6,500 mg / hr, 7,000 mg / hr, 7,500 mg / hr, 8,000 mg / hr, 8,500 mg / hr, 9,000 mg / hr, 9,500 mg / hr, 10,000 mg / hr, 20,000 mg / hr, 30,000 mg / hr, 40,000 mg / hr, 50,000 mg / hr, 60,000 mg / hr, 70,000 mg / hr, 80,000 mg / hr, 90,000 mg / hr, 100,000 mg / hr, 110,000 mg / hr, or 120,000 mg / hr.

[0188] In some embodiments, the lithium-rich intermediate electrode comprises at least 10 atomic % (at%), 12 at%, 14 at%, 16 at%, 18 at%, 20 at%, 22 at%, 24 at%, 26 at%, 28 at%, 30 at%, 32 at%, 34 at%, 36 at%, 38 at%, 40 at%, 42 at%, 44 at%, 46 at%, 48 at%, 50 at%, 52 at%, 54 at%, 56 at%, 58 at%, or 60 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 10 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 12 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 14 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 16 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 18 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 20 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 22 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 24 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 26 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 28 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 30 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 32 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 34 at% more than a minimum amount of lithium that can be present. In some embodiments, thelithium-rich intermediate electrode comprises at least 36 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 38 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 40 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 42 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 44 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 46 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 48 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 50 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 52 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 54 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 56 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 58 at% more than a minimum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at least 60 at% more than a minimum amount of lithium that can be present.

[0189] In some embodiments, the lithium-rich intermediate electrode comprises at least 10 mole%, 12 mole%, 14 mole%, 16 mole%, 18 mole%, 20 mole%, 22 mole%, 24 mole%, 26 mole%, 28 mole%, 30 mole%, 32 mole%, 34 mole%, 36 mole%, 38 mole%, 40 mole%, 42 mole%, 44 mole%, 46 mole%, 48 mole%, 50 mole%, 52 mole%, 54 mole%, 56 mole%, 58 mole%, or 60 mole% more than a minimum amount of lithium that can be present.

[0190] In some embodiments, the lithium-rich intermediate electrode comprises at most 10 atomic % (at%), 12 at%, 14 at%, 16 at%, 18 at%, 20 at%, 22 at%, 24 at%, 26 at%, 28 at%, 30 at%, 32 at%, 34 at%, 36 at%, 38 at%, 40 at%, 42 at%, 44 at%, 46 at%, 48 at%, 50 at%, 52 at%, 54 at%, 56 at%, 58 at%, or 60 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 10 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 12 at% of a maximum amount of lithium that can be present. Insome embodiments, the lithium-rich intermediate electrode comprises at most 14 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 16 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 18 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 20 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 22 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 24 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 26 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 28 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 30 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 32 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 34 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 36 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 38 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 40 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 42 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 44 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 46 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 48 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 50 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 52 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 54 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 56 at% of a maximum amount of lithium that can bepresent. In some embodiments, the lithium-rich intermediate electrode comprises at most 58 at% of a maximum amount of lithium that can be present. In some embodiments, the lithium-rich intermediate electrode comprises at most 60 at% of a maximum amount of lithium that can be present.

[0191] In some embodiments, the lithium-rich intermediate electrode comprises at most 10 mole%, 12 mole%, 14 mole%, 16 mole%, 18 mole%, 20 mole%, 22 mole%, 24 mole%, 26 mole%, 28 mole%, 30 mole%, 32 mole%, 34 mole%, 36 mole%, 38 mole%, 40 mole%, 42 mole%, 44 mole%, 46 mole%, 48 mole%, 50 mole%, 52 mole%, 54 mole%, 56 mole%, 58 mole%, or 60 mole% of a maximum amount of lithium that can be present.

[0192] In some embodiments, a process of (iii) can be performed by applying an electric potential across the lithium-rich intermediate electrode and the current collector substrate. In some embodiments, the process of (iii) can be performed using an applied potential of at least 3V, 4V, 5V, 6V, 7V, 8V, 9V, 10V, 11V or 12V. In some embodiments, the process of (iii) can be performed using an applied potential of at most 3 V, 4V, 5V, 6V, 7V, 8V, 9V, 10V, 1 IV, or 12V. In some embodiments, the process of (ii) can be performed using an applied potential of about 3V to 12V, 4V to 9V, 5V to 8V, or 6V to 7V. In some embodiments, transferring the lithium from the lithium-rich intermediate electrode to the current collector substrate in (iii) comprises delithiating the lithium from the lithium-rich intermediate electrode.

[0193] In some embodiments, an amount of the lithium transferred from the lithium-rich intermediate electrode to the current collector substrate comprises at least 0.1 mg / hr, 0.5 mg / hr, 1 mg / hr, 5 mg / hr, 10 mg / hr, 50 mg / hr, 100 mg / hr, 150 mg / hr, 200 mg / hr, 250 mg / hr, 300 mg / hr, 350 mg / hr, 400 mg / hr, 450 mg / hr, 500 mg / hr, 550 mg / hr, 600 mg / hr, 650 mg / hr, 700 mg / hr, 750 mg / hr, 800 mg / hr, 850 mg / hr, 900 mg / hr, 950 mg / hr, 1,000 mg / hr, 1,200 mg / hr, 1,400 mg / hr, 1,600 mg / hr, 1,800 mg / hr, 2,000 mg / hr, 2,500 mg / hr, 3,000 mg / hr, 3,500 mg / hr, 4,000 mg / hr, 4,500 mg / hr, 5,000 mg / hr, 5,500 mg / hr, 6,000 mg / hr, 6,500 mg / hr, 7,000 mg / hr, 7,500 mg / hr, 8,000 mg / hr, 8,500 mg / hr, 9,000 mg / hr, 9,500 mg / hr, 10,000 mg / hr, 20,000 mg / hr, 30,000 mg / hr, 40,000 mg / hr, 50,000 mg / hr, 60,000 mg / hr, 70,000 mg / hr, 80,000 mg / hr, 90,000 mg / hr, 100,000 mg / hr, 110,000 mg / hr, or 120,000 mg / hr. In some embodiments, an amount of the lithium transferred from the aqueous source to the intermediate electrode comprises at most 0.1 mg / hr, 0.5 mg / hr, 1 mg / hr, 5 mg / hr, 10 mg / hr, 50 mg / hr, 100 mg / hr, 150 mg / hr, 200 mg / hr, 250 mg / hr, 300 mg / hr, 350 mg / hr, 400 mg / hr, 450 mg / hr, 500 mg / hr, 550 mg / hr, 600 mg / hr, 650 mg / hr, 700 mg / hr, 750 mg / hr, 800 mg / hr, 850 mg / hr, 900 mg / hr, 950 mg / hr, 1,000 mg / hr, 1,200 mg / hr, 1,400 mg / hr, 1,600 mg / hr, 1,800 mg / hr, 2,000 mg / hr, 2,500 mg / hr, 3,000 mg / hr, 3,500 mg / hr,4,000 mg / hr, 4,500 mg / hr, 5,000 mg / hr, 5,500 mg / hr, 6,000 mg / hr, 6,500 mg / hr, 7,000 mg / hr, 7,500 mg / hr, 8,000 mg / hr, 8,500 mg / hr, 9,000 mg / hr, 9,500 mg / hr, 10,000 mg / hr, 20,000 mg / hr, 30,000 mg / hr, 40,000 mg / hr, 50,000 mg / hr, 60,000 mg / hr, 70,000 mg / hr, 80,000 mg / hr, 90,000 mg / hr, 100,000 mg / hr, 110,000 mg / hr, or 120,000 mg / hr.

[0194] In some embodiments, the intercalating of lithium and the delithiating are reversible.

[0195] In some embodiments, the current collector substrate comprises Al, Cu, Ni, Ti, stainless steel, or carbonaceous material. In some embodiments, the current collector substrate comprises Cu-Ni, Cu-Ti, Cu-Zn, Cu-Al, Cu-Sn, Ni-CO, Al-Mg, Fe-Cr-Ni, or any combination thereof In some embodiments, the transferring of the lithium from the lithium-rich intermediate electrode to the current collector substrate comprises electrodeposition of the lithium as a layer of lithium metal on the current collector substrate.

[0196] In some embodiments, a current collector substrate may have a thickness of at least 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 20, 30, 40, 50, 60, 70, 80, 90, 100, 200, 300, 400, 500, 600, 700, 800, 900, or 1000 pm. In some embodiments, a current collector substrate may have a thickness of at most 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 20, 30, 40, 50, 60, 70, 80, 90, 100, 200, 300, 400, 500, 600, 700, 800, 900, or 1000 pm.

[0197] In some embodiments, a current collector substrate comprises copper, stainless steel, aluminum, nickel, titanium, sintered carbon, copper or stainless steel that is surface-treated with carbon, nickel, titanium or silver, and aluminum-cadmium alloys. In some embodiments, a current collector substrate comprises fine irregularities on surfaces thereof so as to enhance adhesive strength of the electrode current collector substrate to the electrode active material.

[0198] In some embodiments, a current collector substrate can comprise various forms including films, sheets, foils, nets, porous structures, foams, and non-woven fabrics. In some embodiments, a current collector substrate comprises carbon, carbon paper, carbon cloth or a metal or noble metal mesh or foil. Derived from the carbonization process of a polymeric precursor such as polyacrylonitrile (PAN) or rayon, carbon cloth is composed of a complex network of pure carbon fibers. High electrical conductivity, high thermal stability, and mechanical strength define the attributes of carbon cloth, making it a suitable material for battery applications. Carbon cloth has resistance to chemical corrosion. High surface area of carbon cloth can promote efficient electron transfer, contributing to high energy and power densities in the lithium batteries. Carbon cloth has porous structure to enhance electrolyte penetration, thereby further increasing the performance metrics of the battery. In addition, carbon cloth offers its light weight andflexibility . Adaptable nature of carbon cloth enables its use in a diverse range of battery configurations, including those requiring bendability or shape conformity.

[0199] In some embodiments, a thickness of the lithium metal layer on the current collector substrate can be at least 1, 2, 3, 4, 5, 6, 7, 8, 9, or 10 pm. In some embodiments, a thickness of the lithium metal layer on the current collector substrate can be at least 1, 5, 10, 20, 30, 40, 50, 100, 200, 300, 400, or 500 pm. In some embodiments, a thickness of the lithium metal layer on the current collector substrate can be at most 1, 5, 10, 20, 30, 40, 50, 100, 200, 300, 400, or 500 pm. In some embodiments, a thickness of the lithium metal layer on the current collector substrate can be about from 1 to 380 pm, from 1 to 370 pm, from 1 to 360 pm, from 1 to 350 pm, from 1 to 340 pm, from 1 to 330 pm, from 1 to 320 pm, from 1 to 310 pm, from 1 to 300 pm, from 1 to 250 pm, from 1 to 200 pm, from 1 to 150 pm, from 1 to 100 pm, from 1 to 90 pm, from 1 to 80 pm, from 1 to 70 pm, from 1 to 60 pm, from 1 to 50 pm, from 1 to 45 pm, from 1 to 40 pm, from 1 to 35 pm, from 1 to 30 pm, from 1 to 25 pm, from 1 to 20 pm, from 1 to 15 pm, from 1 to 10 pm, or from 1 to 5 pm.

[0200] Term, Sp refers to the maximum peak height, or the largest individual deviation of a peak from the mean plane. In the present disclosure, the largest single bump or defect on the lithium metal surface extends at most 1.2 micron (pm) above the average surface level. In the present disclosure, the largest single bump or defect on the lithium metal surface extends at most 2 micron (pm) above the average surface level. In some embodiments, the measurements of surface roughness can be conducted by a profilometer. The measurements of surface roughness are shown in FIG. 10. In the present disclosure, the largest single bump or defect on the lithium metal surface extends at most 4 micron (pm) above the average surface level. In some embodiments, the lithium metal layer on the current collector substrate has a 0.5 pm, 1 pm, 1.1 pm, 1.2 pm, 1.3 pm, 1.4 pm, 1.5 pm, 1.6 pm, 1.7 pm, 1.8 pm, 1.9 pm, 2 pm, 2.1 pm, 2.2 pm, 2.3 pm, 2.4 pm, 2.5 pm, 3 pm, 3.5 pm, 4 pm, 4.5 pm, 5 pm, 5.5 pm, 6 pm, 6.5 pm, 7 pm, 7.5 pm, 8 pm, 8.5 pm, 9 pm, 9.5 pm, or 10 pm defect (Sp). In some embodiments, the lithium metal layer on the current collector substrate has an about 0.5 pm, about 0.6 pm, about 0.7 pm, about 0.8 pm, about 0.9 pm, about 1 pm, about 1.1 pm, about 1.2 pm, about 1.3 pm, about 1.4 pm, about 1.5 pm, about 1.6 pm, about 1.7 pm, about 1.8 pm, about 1.9 pm, about 2 pm, about 2.1 pm, about 2.2 pm, about 2.3 pm, about 2.4 pm, about 2.5 pm, about 3 pm, about 3.5 pm, about 4 pm, about 4.5 pm, about 5 pm, about 5.5 pm, about 6 pm, about 6.5 pm, about 7 pm, about 7.5 pm, about 8 pm, about 8.5 pm, about 9 pm, about 9.5 pm, or about 10 pm defect (Sp). Insome embodiments, the lithium metal layer on the current collector substrate has an at least 0.5 pm, at least 0.6 pm, at least 0.7 pm, at least 0.8 pm, at least 0.9 pm, at least 1 pm, at least 1.1 pm, at least 1.2 pm, at least 1.3 pm, at least 1.4 pm, at least 1.5 pm, at least 1.6 pm, at least 1.7 pm, at least 1.8 pm, at least 1.9 pm, at least 2 pm, at least 2.1 pm, at least 2.2 pm, at least 2.3 pm, at least 2.4 pm, at least 2.5 pm, at least 3 pm, at least 3.5 pm, at least 4 pm, at least 4.5 pm, at least 5 pm, at least 5.5 pm, at least 6 pm, at least 6.5 pm, at least 7 pm, at least 7.5 pm, at least 8 pm, at least 8.5 pm, at least 9 pm, at least 9.5 pm, or at least 10 pm defect (Sp). In some embodiments, the lithium metal layer on the current collector substrate has an at most 0.5 pm, at most 0.6 pm, at most 0.7 pm, at most 0.8 pm, at most 0.9 pm, at most 1 pm, at most 1.1 pm, at most 1.2 pm, at most 1.3 pm, at most 1.4 pm, at most 1.5 pm, at most 1.6 pm, at most 1.7 pm, at most 1.8 pm, at most 1.9 pm, at most 2 pm, at most 2.1 pm, at most 2.2 pm, at most 2.3 pm, at most 2.4 pm, at most 2.5 pm, at most 3 pm, at most 3.5 pm, at most 4 pm, at most 4.5 pm, at most 5 pm, at most 5.5 pm, at most 6 pm, at most 6.5 pm, at most 7 pm, at most 7.5 pm, at most 8 pm, at most 8.5 pm, at most 9 pm, at most 9.5 pm, or 10 pm defect (Sp).

[0201] Term, Sa, refers to the arithmetical mean surface roughness. It is calculated as the average of all absolute distances of the roughness profile from the arithmetic mean line over a given evaluation length or area. It is the average roughness of the entire surface area under consideration. In some embodiments, the measurements of surface roughness can be conducted by a profilometer. The measurements of surface roughness are shown in FIG. 10. In some embodiments, the lithium metal layer on the current collector substrate has an average roughness of at most 0.2 microns (pm) (Sa). In some embodiments, the lithium metal layer on the current collector substrate has an average roughness of at most 1 microns (pm) (Sa). In some embodiments, the lithium metal layer on the current collector substrate has an average roughness of at most 0.5 microns (pm) (Sa). In some embodiments, the lithium metal layer on the current collector substrate has an average roughness of at most 1.6 microns (pm) (Sa). In some embodiments, the lithium metal layer on the current collector substrate has an average roughness of 0.1 microns (pm), 0.12 pm, 0.14 pm, 0.16 pm, 0.18 pm, 0.2 pm, 0.22 pm, 0.24 pm, 0.26 pm, 0.28 pm, 0.3 pm, 0.32 pm, 0.34 pm, 0.36 pm, 0.38 pm, 0.4 pm, 0.45 pm, 0.5 pm, 0.55 pm, 0.6 pm, 0.65 pm, 0.7 pm, 0.75 pm, 0.8 pm, 0.85 pm, 0.9 pm, 0.95 pm, 1 pm, 1.2 pm, 1.4 pm, 1.6 pm, 1.8 pm, or 2 pm (Sa). In some embodiments, the lithium metal layer on the current collector substrate has an average roughness of about 0.1 pm, about 0.12 pm, about 0.14 pm, about 0.16 pm, about 0.18 pm, about 0.2 pm, about 0.22 pm, about 0.24 pm, about 0.26 pm, about 0.28pm, about 0.3 pin, about 0.32 pm, about 0.34 pm, about 0.36 pm, about 0.38 pm, about 0.4 pm, about 0.45 pm, about 0.5 pm, about 0.55 pm, about 0.6 pm, about 0.65 pm, about 0.7 pm, about 0.75 pm, about 0.8 pm, about 0.85 pm, about 0.9 pm, about 0.95 pm, about 1 pm, about 1.2 pm, about 1.4 pm, about 1.6 pm, about 1.8 pm, or about 2 pm (Sa). In some embodiments, the lithium metal layer on the current collector substrate has an average roughness of at least 0.1 pm, at least 0.12 pm, at least 0.14 pm, at least 0.16 pm, at least 0.18 pm, at least 0.2 pm, at least 0.22 pm, at least 0.24 pm, at least 0.26 pm, at least 0.28 pm, at least 0.3 pm, at least 0.32 pm, at least 0.34 pm, at least 0.36 pm, at least 0.38 pm, at least 0.4 pm, at least 0.45 pm, at least 0.5 pm, at least 0.55 pm, at least 0.6 pm, at least 0.65 pm, at least 0.7 pm, at least 0.75 pm, at least 0.8 pm, at least 0.85 pm, at least 0.9 pm, at least 0.95 pm, at least 1 pm, at least 1.2 pm, at least 1.4 pm, at least 1.6 pm, at least 1.8 pm, or at least 2 pm (Sa). In some embodiments, the lithium metal layer on the current collector substrate has an average roughness of at most 0.1 pm, at most 0.12 pm, at most 0.14 pm, at most 0.16 pm, at most 0.18 pm, at most 0.2 pm, at most 0.22 pm, at most 0.24 pm, at most 0.26 pm, at most 0.28 pm, at most 0.3 pm, at most 0.32 pm, at most 0.34 pm, at most 0.36 pm, at most 0.38 pm, at most 0.4 pm, at most 0.45 pm, at most 0.5 pm, at most 0.55 pm, at most 0.6 pm, at most 0.65 pm, at most 0.7 pm, at most 0.75 pm, at most 0.8 pm, at most 0.85 pm, at most 0.9 pm, at most 0.95 pm, at most 1 pm, at most 1.2 pm, at most 1.4 pm, at most 1.6 pm, at most 1.8 pm, or at most 2 pm (Sa).

[0202] A nodule size of the lithium metal layer on the current collector substrate can be highly tunable depending on deposition condition. The measurements of nodule size are shown in FIG.11. In some embodiments, a nodule size of the lithium metal layer on the current collector substrate is 10 pm to 15 pm in diameter. In some embodiments, the measurements of a nodule size can be conducted by a Scanning Electron Microscope (SEM). In some embodiments, a nodule size of the lithium metal layer on the current collector substrate is 1 pm to 40 pm in diameter. In some embodiments, a nodule size of the lithium metal layer on the current collector substrate is 1 pm to 60 pm in diameter. In some embodiments, a nodule size of the lithium metal layer on the current collector substrate is 1 pm, 5 pm, 10 pm, 11 pm, 12 pm, 13 pm, 14 pm, 15 pm, 16 pm, 17 pm, 18 pm, 19 pm, 20 pm, 25 pm, 30 pm, 35 pm, 40 pm, 45 pm, 50 pm, 55 pm, or 60 pm in diameter. In some embodiments, a nodule size of the lithium metal layer on the current collector substrate is about 1 pm, about 5 pm, about 10 pm, about 11 pm, about 12 pm, about 13 pm, about 14 pm, about 15 pm, about 16 pm, about 17 pm, about 18 pm, about 19 pm, about 20 pm, about 25 pm, about 30 pm, about 35 pm, about 40 pm, about 45 pm, about 50 pm,about 55 m, or about 60 pm in diameter. In some embodiments, a nodule size of the lithium metal layer on the current collector substrate is at least 1 pm, at least 5 pm, at least 10 pm, at least 11 pm, at least 12 pm, at least 13 pm, at least 14 pm, at least 15 pm, at least 16 pm, at least 17 pm, at least 18 pm, at least 19 pm, at least 20 pm, at least 25 pm, at least 30 pm, at least 35 pm, at least 40 pm, at least 45 pm, at least 50 pm, at least 55 pm, or at least 60 pm in diameter. In some embodiments, a nodule size of the lithium metal layer on the current collector substrate is at most 1 pm, at most 5 pm, at most 10 pm, at most 11 pm, at most 12 pm, at most 13 pm, at most 14 pm, at most 15 pm, at most 16 pm, at most 17 pm, at most 18 pm, at most 19 pm, at most 20 pm, at most 25 pm, at most 30 pm, at most 35 pm, at most 40 pm, at most 45 pm, at most 50 pm, at most 55 pm, or at most 60 pm in diameter.

[0203] In some embodiments, the prepared electrode is a battery-ready electrode.

[0204] In some embodiments, the battery-ready electrode comprises the lithium metal with an impurity level of less than about 1000, 900, 800, 700, 600, 500, 400, 300, 200, 100, 90, 80, 70, 60, 50, 40, 30, 20, 10, 9, 8, 7, 6, 5, 4, 3, 2, 1, 0.9, 0.8, 0.7, 0.6, 0.5, 0.4, 0.3, 0.2, or 0.1 parts-per- million (ppm) of a non-metallic element. The ppm can be by mass or by count. The ppm can correspond to a basis used for the instrument to detect the non-metallic element. Lithium metal can comprise less than 5 ppm of non-metallic elements. In some embodiments, the lithium metal includes no more than 1 ppm of non-metallic elements by mass. In some embodiments, the lithium metal includes no more than 10 ppm of non-metallic elements by mass. In some embodiments, the lithium metal includes no more than 20 ppm of non-metallic elements by mass. In some embodiments, the lithium metal includes no more than 30 ppm of non-metallic elements by mass. In some embodiments, the lithium metal includes no more than 40 ppm of non-metallic elements by mass. In some embodiments, the lithium metal includes no more than 100 ppm of non-metallic elements by mass. In some embodiments, the lithium metal includes no more than 200 ppm of non-metallic elements by mass. In some embodiments, the lithium metal includes no more than 300 ppm of non-metallic elements by mass. The non-metallic element can be nitrogen, boron, oxygen, carbon, hydrogen, or fluorine. Non-metallic elements can be present as atomic species, or molecular species (e.g., as LisN, OH, lithium-boron compounds, carbonate, or O2). In some embodiments, a non-metallic element can form a resistive material on a surface of the lithium metal. In some embodiments, the layer of lithium metal can comprise less than 0.1 wt% or at% of non-conductive elements or compounds.

[0205] In some embodiments, the battery-ready electrode can comprise a low density of structural impurities, e.g., subsurface structural impurities. Without being bound to a particulartheory, elemental or molecular impurities in lithium metal can form phases that are distinct from the lithium upon cycling. In some embodiments, the electrode can be heated. Higher temperatures can permit impurities to conduct or diffuse in the lithium metal, which can lead to the formation of more stable phases of impurities in the lithium metal (e.g., crystallites). When such structural impurities (phases that have distinct crystal structures, or which have grain boundaries against lithium metal phases in the lithium metal) begin to form, they can continue to grow. Structural impurities can be detected by 3D techniques, e.g., X-ray tomography. Structural impurities can be present on the surface of lithium metal, or they can be present beneath the surface. The structural impurities can provide sites for dendrite nucleation or growth and can crack the surrounding lithium metal. In some embodiments, the lithium metal can comprise less than 10, 9, 8, 7, 6, 5, 4, 3, 2, 1, 0.9, 0.8, 0.7, 0.6, 0.5, 0.4, 0.3, 0.2, or 0.1 structural impurities / mm3. In some embodiments, the lithium metal can comprise less than 1000, 900, 800, 700, 600, 500, 400, 300, 200, 100, 90, 80, 70, 60, 5,0 40, 30, 20, 10, 9, 8, 7, 6, 5, 4, 3, 2, or 1 ppm of structural impurities by weight.

[0206] In some embodiments, after (iii), the current collector with the layer of lithium can be treated by refining or post processes. In some embodiments, the refining or post processes comprise cleaning, heating, or applying pressure on the electrode. In some embodiments, the refining or post processes comprise heating the electrode at a temperature below about 150°C. In some embodiments, the electrode can be further treated by heat at most 100°C, 110°C, 120°C, 130°C, 140°C, 150°C, 160°C, or 170°C as the refining or post processes. In some embodiments, the electrode can be further treated by heat at least 100°C, 110°C, 120°C, 130°C, 140°C, 150°C, or 160°C as the refining or post processes. In some embodiments, the refining or post processes comprise applying pressures on the electrode at most 5 MPa. In some embodiments, the electrode can be further treated by applying pressure at least 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 15, or 20 megapascals (MPa). In some embodiments, the electrode can be further treated by applying pressure at most 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 15, or 20 megapascals (MPa).

[0207] In some embodiments, the processes of (i) and (ii) can be carried out in a first chamber and the process of (iii) can be carried out in a second chamber that is different from the first chamber. In some embodiments, the lithium-rich intermediate electrode can be transported to the second chamber. In some embodiments, the processes of (i), (ii), and (iii) are performed in one chamber. In case of performing in one chamber, after the processes of (i) and (ii), the aqueous source can be replaced by an electrolyte for the process (iii) and a counter electrode can be added to the chamber for the process of (iii).

[0208] In some embodiments, the intermediate electrode can be delithiated after (iii) and returned to the first chamber for repeating (i) and (ii). In some embodiments, the method further comprises, after (iii), re-using the intermediate electrode in (i).

[0209] In some embodiments, after (ii) and before (iii), the intermediate electrode can be rinsed and / or dried.

[0210] In some embodiments, the counter electrode, the intermediate electrode, and / or the current collector substrate are in a roll form. In some embodiments, an electrode rolling press system can be used. In some embodiments, the method can be used for a scale-up production.

[0211] In certain aspects, the present disclosure provides electrochemical methods of lithium extraction from brine and lithium metal deposition. It involves an intermediate electrode / lithium- rich intermediate electrode that serves as a temporary reservoir of lithium. In one embodiment, during the process of extracting lithium from brine, the intermediate electrode can function as a platform for lithium deposition. In another embodiment, the intermediate electrode can serve as a source for transferring lithium onto a current collector substrate. The process of lithium ion transfer onto the substrate transforms the intermediate electrode into a lithium-rich intermediate electrode. The lithium ions from the lithium-rich intermediate electrode are subsequently transferred onto a current collector substrate, resulting in the formation of a lithium-based electrode. This electrode can be suitable for incorporation into a rechargeable energy device, such as a lithium-ion battery.

[0212] In some embodiments, the intermediate electrode can comprise FePC In some instances, the intermediate electrode can be immersed in a brine solution and subjected to an electrochemical lithiation process to produce a lithium-rich intermediate electrode comprising LiFePCU. Following the lithiation process, the lithium-rich intermediate electrode comprising LiFePC can be used to transfer lithium ions onto a current collector substrate, thereby creating a lithium metal electrode enriched with high-purity lithium.

[0213] In certain embodiments, the process described herein does not necessitate cleaning or drying stages in the preparation of the high-purity lithium metal electrode, largely due to the inclusion of a separator between the intermediate electrode and the current collector substrate. The separator comprises a lithium-ion selective membrane that selectively permits the passage of lithium ions while inhibiting the transfer of undesired contaminants such as organic solvents, anions of lithium salts, and water. This lithium-ion selective membrane can provide an effective barrier to prevent the transfer of lithium-reactive components, such as non-lithium ions or solvents, from the counter electrode side to the intermediate electrode side.

[0214] In certain aspects, the present disclosure provides a method for producing lithium iron phosphate (LFP) from an aqueous source comprising lithium. In some embodiments, the aqueous source comprising lithium comprises brine. The method can involve a couple of stages. The first step can involve the production of lithium phosphate (LP) from brine. The second step can involve using the LP as a source material for the synthesis of LFP. This two-step procedure, from concentrating brine to precipitate LP, and subsequently using the LP to synthesize LFP, demonstrates a viable and sustainable approach to LFP production.

[0215] In some embodiments, the first step focuses on the production of LP from the brine solution. This can be achieved by subjecting the brine to an electrical process, particularly electrodialysis. This process applies a voltage across the brine solution, migrating lithium ions through a lithium ion-selective membrane, which results in their concentration in a separate compartment. Once the lithium ions are concentrated using electrodialysis, in some embodiments, a phosphate source can be added to the concentrated lithium ion solution to precipitate lithium phosphate. This can involve adjusting the pH of the solution, which causes the lithium phosphate to precipitate out of the solution. The precipitated lithium phosphate can then be separated and collected. The precipitated LP can be combined with a source of iron ions, such as iron (II) sulfate, in a suitable solvent to create an electrolyte solution. Subsequently, a substrate electrode can be immersed into the combined solution, and an electric potential can be applied across the solution. Under the applied electric field, the lithium, iron, and phosphate ions migrate towards the substrate electrode to electrodeposit as LFP on the substrate.

[0216] In some embodiments, the first step can be achieved through a process of concentration, where the brine is subjected to specific conditions that facilitate the precipitation of LP. By focusing on the concentration and precipitation process, the LP can be isolated from the brine, yielding high-quality LP. The concentration of brine can be carried out by various methods. In some embodiments, natural evaporation can be used. It can involve exposing the brine to air and sunlight in large shallow ponds, allowing the water to evaporate and the minerals to concentrate. In some embodiments, solar evaporation can be used as an enhanced method such as solar concentrators to speed up the evaporation process. In some embodiments, vacuum evaporation can be used to lower the boiling point of the water in the brine, causing it to evaporate at a lower temperature and thus save energy. In some embodiments, membrane processes can be used. As a unlimited example, semi-permeable membranes can be used to separate the water from the brine. Reverse osmosis and nanofiltration are two common types of membrane processes. After the concentration step, lithium phosphate can be precipitated out of the solution. This can be done bychanging the pH of the brine, by adding a suitable reagent that reacts with the lithium to form lithium phosphate. The precipitate can be separated from the solution, by filtration or centrifugation.

[0217] In some embodiments, the first step can be accomplished via an electrodialysis. Electrodialysis is a membrane process in which ions are transported through a semi-permeable membrane under the influence of an electric potential. By applying a voltage across the brine solution, the migration of lithium ions can be induced through a selective membrane, effectively concentrating them in a separate compartment. In some embodiments, the selective membrane can comprise a series of anion and cation exchange membranes, assembled alternately, between two electrodes. These membranes are permeable to ions of opposite charge. When a direct current is applied across the setup, lithium ions are attracted towards the cathode (the negatively charged electrode). They move through the cation exchange membranes but are blocked by the anion exchange membranes. This causes the lithium ions to become concentrated in compartments between the cation exchange membranes and the anion exchange membranes. The compartments between the anion exchange membranes and the cation exchange membranes, on the other hand, become depleted in lithium ions. This results in two streams: one that is concentrated in lithium ions, and one that is depleted.

[0218] Once the lithium ions are concentrated, in some embodiments, a phosphate source can be added to the concentrated lithium ion solution to precipitate lithium phosphate. This can involve adjusting the pH of the solution, which causes the lithium phosphate to precipitate out of the solution. The precipitated lithium phosphate can then be separated and collected. Various phosphate sources can be used to precipitate lithium phosphate from a concentrated lithium solution. The phosphate sources include, but not limited to sodium phosphate (NasPCU), ammonium phosphate ((NH^PCU), phosphoric acid (H3PO4), and calcium phosphate (Ca3(PO4)2). The phosphate sources should not introduce additional ions into the solution, which could potentially interfere with the precipitation process or contaminate the lithium phosphate product.

[0219] In some embodiments, the production of LFP from the concentrated lithium solution can undergo the process of the electrochemical deposition. In this process, a solution can be prepared comprising a source of iron ions, for example iron (II) sulfate, and phosphate ions, for example phosphoric acid. The solution can be combined with the concentrated lithium solution from the first step. The mixing of the two solutions provides a mixed solution comprising lithium, iron, and phosphate ions. Following the mixing of the solutions, a substrate electrode can be immersedinto the combined solution. An electric potential can be applied across the combined solution to instigate the migration of lithium, iron, and phosphate ions towards the substrate electrode to form lithium iron phosphate, which precipitates out of the solution and deposits onto the substrate electrode.SYSTEMS

[0220] In certain aspects, this disclosure also provides a system for preparing an electrode. In some embodiments, the system comprises a first chamber and a second chamber. In some embodiments, the first chamber comprises an aqueous source comprising lithium and an intermediate electrode. In some embodiments, the intermediate electrode is configured to extract and receive the lithium from the aqueous source to form a lithium-rich intermediate electrode. In some embodiments, the second chamber comprises a current collector substrate. In some embodiments, the lithium-rich intermediate electrode is configured to be transferred from the first chamber to the second chamber. In some embodiments, the lithium from the lithium-rich intermediate electrode is transferred to the current collector substrate to form an electrode for a rechargeable energy device.

[0221] In some embodiments, the aqueous source comprising lithium is brine. In some embodiments, the aqueous source comprising lithium further comprises Na+, K+, Mg2+, Ca2+, B(OH)4, Fe2+, Fe3+, Mn2+, MnO , MnO4, Cl’, SO42’, NH3, NH4+, NH40H, NO2, HN02, NO3’, an alkali metal ions, an alkali earth metal ions, or any combination thereof. In some embodiments, the aqueous source comprising lithium comprises a geological resource. In some embodiments, the aqueous source comprising lithium can be pretreated to remove Na+, K+, Mg2+, Ca2+, B(OH)4, Fe2+, Fe3+, Mn2+, MnO42, MnO4, CF, SO42’, NH3, NH4+, NH40H, NO2, HN02, NO3‘, an alkali metal ions, an alkali earth metal ions, or any combination thereof.

[0222] In some embodiments, the system further comprises a counter electrode that is electrically connected with the intermediate electrode in a circuit, using the aqueous source comprising lithium as an electrolyte. In some embodiments, the counter electrode comprises graphite, platinum (Pt), titanium (Ti), or a combination thereof.

[0223] In some embodiments of the present disclosure, the electrode can be a negative electrode. A negative electrode refers to the electrode that is negatively charged during the charging of a rechargeable battery, and positively charged during the discharging of a rechargeable battery. The negative electrode can refer to the electrode where a reduction half-reaction occurs during charging, and an oxidation half-reaction occurs during discharging.

[0224] In some embodiments, the electrode can be a positive electrode. A positive electrode can refer to the electrode that is positively charged during the charging of a rechargeable battery, and positively charged during the discharging of a rechargeable battery. The positive electrode can refer to the electrode where an oxidation half-reaction occurs during charging, and a reduction half-reaction occurs during discharging.

[0225] In some embodiments, a width of the electrode comprises 50 mm, 60 mm, 70 mm, 80 mm, 90 mm, 100 mm, 110 mm, 120 mm, 130 mm, 140 mm, 150 mm, 160 mm, 170 mm, 180 mm, 190 mm, 200 mm, 210 mm, 220 mm, 230 mm, 240 mm, 250 mm, 260 mm, 270 mm, 280 mm, 290 mm, 300 mm, 310 mm, 320 mm, 330 mm, 340 mm, 350 mm, 360 mm, 370 mm, 380 mm, 390 mm, 400 mm, 410 mm, 420 mm, 430 mm, 440 mm, 450 mm, 460 mm, 470 mm, 480 mm, 490 mm, 500 mm, 510 mm, 520 mm, 530 mm, 540 mm, 550 mm, 560 mm, 570 mm, 580 mm, 590 mm, 600 mm, 610 mm, 620 mm, 630 mm, 640 mm, 650 mm, 660 mm, 670 mm, 680 mm, 690 mm, 700 mm, 710 mm, 720 mm, 730 mm, 740 mm, 750 mm, 760 mm, 770 mm, 780 mm, 790 mm, 800 mm, 810 mm, 820 mm, 830 mm, 840 mm, 850 mm, 860 mm, 870 mm, 880 mm, 890 mm, 900 mm, 910 mm, 920 mm, 930 mm, 940 mm, 950 mm, 960 mm, 970 mm, 980 mm, 990 mm, 1000 mm, 1100 mm, 1200 mm, 1300 mm, 140 mm, or 1500 mm. In some embodiments, a width of the electrode comprises about 50 mm, about 60 mm, about 70 mm, about 80 mm, about 90 mm, about 100 mm, about 110 mm, about 120 mm, about 130 mm, about 140 mm, about 150 mm, about 160 mm, about 170 mm, about 180 mm, about 190 mm, about200 mm, about 210 mm, about 220 mm, about 230 mm, about 240 mm, about 250 mm, about260 mm, about 270 mm, about 280 mm, about 290 mm, about 300 mm, about 310 mm, about320 mm, about 330 mm, about 340 mm, about 350 mm, about 360 mm, about 370 mm, about380 mm, about 390 mm, about 400 mm, about 410 mm, about 420 mm, about 430 mm, about440 mm, about 450 mm, about 460 mm, about 470 mm, about 480 mm, about 490 mm, about500 mm, about 510 mm, about 520 mm, about 530 mm, about 540 mm, about 550 mm, about560 mm, about 570 mm, about 580 mm, about 590 mm, about 600 mm, about 610 mm, about620 mm, about 630 mm, about 640 mm, about 650 mm, about 660 mm, about 670 mm, about680 mm, about 690 mm, about 700 mm, about 710 mm, about 720 mm, about 730 mm, about740 mm, about 750 mm, about 760 mm, about 770 mm, about 780 mm, about 790 mm, about800 mm, about 810 mm, about 820 mm, about 830 mm, about 840 mm, about 850 mm, about860 mm, about 870 mm, about 880 mm, about 890 mm, about 900 mm, about 910 mm, about920 mm, about 930 mm, about 940 mm, about 950 mm, about 960 mm, about 970 mm, about980 mm, about 990 mm, about 1000 mm, about 1100 mm, about 1200 mm, about 1300 mm,about 140 mm, or about 1500 mm. In some embodiments, a width of the electrode comprises at least 50 mm, 60 mm, 70 mm, 80 mm, 90 mm, 100 mm, 110 mm, 120 mm, 130 mm, 140 mm, 150 mm, 160 mm, 170 mm, 180 mm, 190 mm, 200 mm, 210 mm, 220 mm, 230 mm, 240 mm,250 mm, 260 mm, 270 mm, 280 mm, 290 mm, 300 mm, 310 mm, 320 mm, 330 mm, 340 mm,350 mm, 360 mm, 370 mm, 380 mm, 390 mm, 400 mm, 410 mm, 420 mm, 430 mm, 440 mm,450 mm, 460 mm, 470 mm, 480 mm, 490 mm, 500 mm, 510 mm, 520 mm, 530 mm, 540 mm,550 mm, 560 mm, 570 mm, 580 mm, 590 mm, 600 mm, 610 mm, 620 mm, 630 mm, 640 mm,650 mm, 660 mm, 670 mm, 680 mm, 690 mm, 700 mm, 710 mm, 720 mm, 730 mm, 740 mm,750 mm, 760 mm, 770 mm, 780 mm, 790 mm, 800 mm, 810 mm, 820 mm, 830 mm, 840 mm,850 mm, 860 mm, 870 mm, 880 mm, 890 mm, 900 mm, 910 mm, 920 mm, 930 mm, 940 mm,950 mm, 960 mm, 970 mm, 980 mm, 990 mm, 1000 mm, 1100 mm, 1200 mm, 1300 mm, 140 mm, or 1500 mm. In some embodiments, a width of the electrode comprises at most 50 mm, 60 mm, 70 mm, 80 mm, 90 mm, 100 mm, 110 mm, 120 mm, 130 mm, 140 mm, 150 mm, 160 mm, 170 mm, 180 mm, 190 mm, 200 mm, 210 mm, 220 mm, 230 mm, 240 mm, 250 mm, 260 mm,270 mm, 280 mm, 290 mm, 300 mm, 310 mm, 320 mm, 330 mm, 340 mm, 350 mm, 360 mm,370 mm, 380 mm, 390 mm, 400 mm, 410 mm, 420 mm, 430 mm, 440 mm, 450 mm, 460 mm,470 mm, 480 mm, 490 mm, 500 mm, 510 mm, 520 mm, 530 mm, 540 mm, 550 mm, 560 mm,570 mm, 580 mm, 590 mm, 600 mm, 610 mm, 620 mm, 630 mm, 640 mm, 650 mm, 660 mm,670 mm, 680 mm, 690 mm, 700 mm, 710 mm, 720 mm, 730 mm, 740 mm, 750 mm, 760 mm,770 mm, 780 mm, 790 mm, 800 mm, 810 mm, 820 mm, 830 mm, 840 mm, 850 mm, 860 mm,870 mm, 880 mm, 890 mm, 900 mm, 910 mm, 920 mm, 930 mm, 940 mm, 950 mm, 960 mm,970 mm, 980 mm, 990 mm, 1000 mm, 1100 mm, 1200 mm, 1300 mm, 140 mm, or 1500 mm.

[0226] In some embodiments, a length of the electrode comprises 50 mm, 100 mm, 200 mm, 300 mm, 400 mm, 500 mm, 600 mm, 700 mm, 800 mm, 900 mm, 1000 mm, 2000 mm, 3000 mm, 4000 mm, or 5000 mm. In some embodiments, a length of the electrode comprises about 50 mm, about 100 mm, about 200 mm, about 300 mm, about 400 mm, about 500 mm, about 600 mm, about 700 mm, about 800 mm, about 900 mm, about 1000 mm, about 2000 mm, about 3000 mm, about 4000 mm, or about 5000 mm. In some embodiments, a length of the electrode comprises at least 50 mm, at least 100 mm, at least 200 mm, at least 300 mm, at least 400 mm, at least 500 mm, at least 600 mm, at least 700 mm, at least 800 mm, at least 900 mm, at least 1000 mm, at least 2000 mm, at least 3000 mm, at least 4000 mm, or at least 5000 mm. In some embodiments, a length of the electrode comprises at most 50 mm, at most 100 mm, at most 200 mm, at most 300 mm, at most 400 mm, at most 500 mm, at most 600 mm, at most 700 mm, at most 800 mm,at most 900 mm, at most 1000 mm, at most 2000 mm, at most 3000 mm, at most 4000 mm, or at most 5000 mm.

[0227] In some embodiments, the intermediate electrode can be a negative electrode. In some embodiments, the intermediate electrode is substantially free of lithium. In some embodiments, the intermediate electrode is in a de-lithiated state. In some embodiments, the intermediate electrode comprises about 60 atomic % (at%), 58 at%, 56 at%, 54 at%, 52 at%, 50 at%, 48 at%, 46 at%, 44 at%, 42 at%, 40 at%, 38 at%, 36 at%, 34 at%, 32 at%, 30 at%, 28 at%, 26 at%, 24 at%, 22 at%, 20 at%, 18 at%, 16 at%, 14 at%, 12 at%, or 10 at% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 60 at%, 58 at%, 56 at%, 54 at%, 52 at%, 50 at%, 48 at%, 46 at%, 44 at%, 42 at%, 40 at%, 38 at%, 36 at%, 34 at%, 32 at%, 30 at%, 28 at%, 26 at%, 24 at%, 22 at%, 20 at%, 18 at%, 16 at%,14 at%, 12 at%, or 10 at% of a maximum amount of lithium that can be present.

[0228] In some embodiments, the intermediate electrode comprises about 60 mole%, 58 mole%, 56 mole%, 54 mole%, 52 mole%, 50 mole%, 48 mole%, 46 mole%, 44 mole%, 42 mole%, 40 mole%, 38 mole%, 36 mole%, 34 mole%, 32 mole%, 30 mole%, 28 mole%, 26 mole%, 24 mole%, 22 mole%, 20 mole%, 18 mole%, 16 mole%, 14 mole%, 12 mole%, or 10 mole% less than a maximum amount of lithium that can be present. In some embodiments, the intermediate electrode comprises at least 60 mole%, 58 mole%, 56 mole%, 54 mole%, 52 mole%, 50 mole%, 48 mole%, 46 mole%, 44 mole%, 42 mole%, 40 mole%, 38 mole%, 36 mole%, 34 mole%, 32 mole%, 30 mole%, 28 mole%, 26 mole%, 24 mole%, 22 mole%, 20 mole%, 18 mole%, 16 mole%, 14 mole%, 12 mole%, or 10 mole% of a maximum amount of lithium that can be present.

[0229] In some embodiments, the intermediate electrode is non-reactive with non-lithium components in the aqueous source.

[0230] In some embodiments, the intermediate electrode is reactive with non-lithium components in the aqueous source. In that case, the intermediate electrode and a nonaqueous / polymer electrolyte are physically separated from a counter (positive) electrode and the aqueous source comprising lithium by a lithium ion-selective membrane. The lithium ion- selective membrane permits lithium ions to flow through to the intermediate electrode selectively. In some embodiments, the lithium ion-selective membrane can substantially prevent or inhibit the passage of organic solvents, anions of lithium salts, water, or a contaminant from being transferred between the intermediate electrode and the counter (positive) electrode. The membrane can prevent the passage of lithium-reactive components (e.g., non-lithium ions, orsolvents) from the counter (positive) electrode side to the intermediate electrode side, to prevent or inhibit the formation of a solid electrolyte interphase. In some embodiments, the lithium ion- selective membrane comprises a single layer or multiple layers. In some embodiments, the lithium ion-selective membrane comprises glass fiber, polyester, polyethylene, polypropylene, polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), and a combination thereof. In some embodiments, the lithium ion-selective membrane comprises hydrophobic polymers. In some embodiments, the lithium ion-selective membrane comprises lithium-ion conductive channels. The lithium ion-selective membrane allows lithium ions to pass between the first chamber and the second chamber, but precludes the passage of other chemical species between the two chambers. In particular, the lithium ion-selective membrane does not allow water to pass from the first chamber to the second chamber.

[0231] In some embodiments, lithium from the aqueous source is extracted and transferred to the intermediate electrode. In some embodiments, transferring lithium to the intermediate electrode comprises intercalating the lithium in the intermediate electrode to form the lithium-rich intermediate electrode. In some embodiments, the lithium-rich electrode is transported from the first chamber to the second chamber.

[0232] In some embodiments, an electric potential is applied across the lithium-rich intermediate electrode and the current collector substrate to transfer the lithium from the lithium-rich intermediate electrode to the current collector substrate to form an electrode. In some embodiments, transferring the lithium from the lithium-rich intermediate electrode to the current collector substrate comprises delithiating the lithium-rich intermediate electrode. In some embodiments, the transferring of the lithium from the lithium-rich intermediate electrode to the current collector substrate comprises electrodeposition of the lithium as a layer of lithium metal on the current collector substrate.

[0233] In some embodiments, the delithiated (previously lithium-rich) intermediate electrode is returned to the first chamber for repeating the same processes.

[0234] In some embodiments, the counter electrode, the intermediate electrode, and / or the current collector substrate are in a roll form. In some embodiments, an electrode rolling press system can be used.

[0235] In some embodiments, the system can comprise three tanks. In some embodiments, referring to FIG. 2, the three tanks comprise a first tank (tank A), a second tank (tank B), and a third tank (thank C). In some embodiments, the first tank (tank A), the second tank (tank B), and the third tank (thank C) comprise a first electrode (electrode 1), a second electrode (electrode 2),and a third electrode (electrode 3), respectively. In some embodiments, the first tank and the second tank are separated by a separator. In some embodiments, the second tank and the third tank are separated by a separator. In some embodiments, the separator comprises a lithium ion- selective membrane. In some embodiments, the lithium ion-selective membrane comprises a single layer or multiple layers. In some embodiments, the lithium ion-selective membrane comprises glass fiber, polyester, polyethylene, polypropylene, polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), and a combination thereof. In some embodiments, the lithium ion-selective membrane comprises hydrophobic polymers. In some embodiments, the lithium ion-selective membrane comprises lithium-ion conductive channels.

[0236] In some embodiments, the first tank comprises an aqueous electrolyte. In some embodiments, the aqueous electrolyte comprises an aqueous source comprising lithium. In some embodiments, the electrolyte is brine. In some embodiments, the electrolyte comprises a lithium salt. In some embodiments, the aqueous source comprising lithium comprises a geological resource. In some embodiments, the aqueous source comprising lithium can be pretreated to remove magnesium, sodium, calcium, potassium, iron, boron, manganese, or any combination thereof.

[0237] In some embodiments, the first tank comprises the first electrode. In some embodiments, electrode 1 can be a counter electrode. In some embodiments, the first electrode can be an anode that generates evolution of gas, for example Ch or Ch. In some embodiments, the first electrode comprises graphite, platinum (Pt), titanium (Ti), or a combination thereof. In some embodiments, the first electrode can be a solid feedstock of lithium. In some embodiments, the first electrode comprises black mass produced from the shredding of lithium-ion battery materials, for example, LiB black mass.

[0238] In some embodiments, the second tank comprises an aqueous electrolyte. In some embodiments, the second tank comprises a nonaqueous electrolyte. In some embodiments, the electrolyte is a polymer electrolyte. In some embodiments, the electrolyte is an organic electrolyte. In some embodiments, the electrolyte comprises a lithium salt. In some embodiments, the electrolyte comprises an ionic liquid. In some embodiments, the electrolyte comprises a deep eutectic solvent.

[0239] In some embodiments, the second tank comprises the second electrode. In some embodiments, the second electrode can be an intermediate electrode. In some embodiments, the second electrode can be a cathode. In some embodiments, the intermediate electrode comprises a metal current collector or a carbon current collector. In some embodiments, the intermediateelectrode comprises a metal current collector. In some embodiments, the metal current collector comprises copper (Cu), titanium (Ti), aluminum (Al), magnesium (Mg), zinc (Zn), tin (Sn), or any metal that is capable of forming an alloy with lithium. In some embodiments, the metal current collector substrate comprises Cu-Ni, Cu-Ti, Cu-Zn, Cu-Al, Cu-Sn, Ni-CO, Al-Mg, Fe- Cr-Ni, or any combination thereof In some embodiments, the current collector comprises vanadium oxide (V2O5). In some embodiments, the current collector comprises metal oxide. In some embodiments, the intermediate electrode comprises a carbon current collector. In some embodiments, the carbon current collector comprises graphite. In some embodiments, the metal current collector comprises copper, aluminum, graphite-coated copper, nickel, silicon, silver, carbon (e.g., rough-surface carbon, graphene), a lithophilic material, aluminum, gold, a copper alloy (Cu-Zn, Cu-Al, Cu-Sn), or any combination thereof. In some embodiments, the intermediate electrode comprises a lithium absorption electrode comprising graphite or metals that alloy with lithium. In some embodiments, the intermediate electrode comprises an electrically conductive slurry comprising an electrically conductive additive. In some embodiments, the electrically conductive additive comprises carbon. In some embodiments, the intermediate electrode comprises black mass produced from the shredding of lithium-ion battery materials, for example LiB black mass.

[0240] In some embodiments, the second electrode can be an anode. In some embodiments, the second electrode can be a lithium-rich intermediate electrode. In some embodiments, the lithium- rich intermediate electrode comprises lithium iron phosphate (LiFePCU, LFP), lithium nickel manganese cobalt oxide (LiNiMnCoCh, NMC), lithium manganate (Li2MnO4, LMO), LiCe, LixMgy, LixAly, LixSiy, or a combination thereof.

[0241] In some embodiments, the third tank comprises an aqueous electrolyte. In some embodiments, the third tank comprises a nonaqueous electrolyte. In some embodiments, the third tank comprises an electrolyte that has been purified. In some embodiments, the electrolyte is a polymer electrolyte. In some embodiments, the electrolyte is an organic electrolyte. In some embodiments, the electrolyte comprises a lithium salt. In some embodiments, the electrolyte comprises an ionic liquid. In some embodiments, the electrolyte comprises a deep eutectic solvent.

[0242] In some embodiments, the third tank comprises the third electrode. In some embodiments, the third electrode can be a cathode. In some embodiments, the third electrode comprises a current collector substrate. In some embodiments, the current collector substrate comprises Al, Cu, Ni, Ti, stainless steel, or carbonaceous material. In some embodiments, thecurrent collector substrate comprises Cu-Ni, Cu-Ti, Cu-Zn, Cu-Al, Cu-Sn, Ni-CO, Al-Mg, Fe- Cr-Ni, or any combination thereof. In some embodiments, a current collector substrate comprises copper, stainless steel, aluminum, nickel, titanium, sintered carbon, copper or stainless steel that is surface-treated with carbon, nickel, titanium or silver, and aluminum-cadmium alloys. In some embodiments, a current collector substrate comprises fine irregularities on surfaces thereof so as to enhance adhesive strength of the electrode current collector substrate to the electrode active material.

[0243] In some embodiments, a current collector substrate can comprise various forms including films, sheets, foils, nets, porous structures, foams, and non-woven fabrics. In some embodiments, a current collector substrate comprises carbon, carbon paper, carbon cloth or a metal or noble metal mesh or foil.

[0244] In some embodiments, the third electrode comprises a metal current collector or a carbon current collector. In some embodiments, the third electrode comprises a metal current collector. In some embodiments, the metal current collector comprises copper (Cu), titanium (Ti), aluminum (Al), magnesium (Mg), zinc (Zn), tin (Sn), or any metal that is capable of forming an alloy with lithium. In some embodiments, the current collector comprises vanadium oxide (V2O5). In some embodiments, the current collector comprises metal oxide. In some embodiments, the third electrode comprises a carbon current collector. In some embodiments, the carbon current collector comprises graphite. In some embodiments, the metal current collector comprises copper, aluminum, graphite-coated copper, nickel, silicon, silver, carbon (e.g., rough-surface carbon, graphene), a lithophilic material, aluminum, gold, a copper alloy (Cu-Zn, Cu-Al, Cu-Sn), or any combination thereof. In some embodiments, the third electrode comprises a lithium absorption electrode comprising graphite or metals that alloy with lithium. In some embodiments, the third electrode comprises an electrically conductive slurry comprising an electrically conductive additive. In some embodiments, the electrically conductive additive comprises carbon.

[0245] Referring to FIG. 2, when an electric potential is applied across the first electrode and the second electrode, lithium can be extracted and transferred from the first electrode (or brine) to the second electrode. In some embodiments, an electric circuit that is connected between the first electrode and the second electrode and can allow a reduction reaction at the second electrode (the intermediate electrode) and an oxidation reaction at the first electrode. In some embodiments, the oxidation reaction at the first electrode comprises evolving a gas comprising oxygen or chlorine.In some embodiments, two or more reactions can be used for the extraction of lithium from a lithium rich, low-purity feedstock, for example, as below (reaction 1).First Electrode (electrode 1; anode):2H2O O2+ 4H++ 4eSecond Electrode (electrode 2; cathode; an intermediate electrode):Li++ e + MPO4 LiMPCE

[0246] Referring to FIG. 2 again, when an electric circuit is connected between the second electrode (a lithium-rich intermediate electrode) and the third electrode, an oxidation reaction can occur at the second electrode, and a reduction reaction can occur at the third electrode to produce a battery-ready electrode, for example, as below (reaction 2).Second Electrode (electrode 2; anode; a lithium-rich intermediate electrode):LiMPCU -^Li + e + MP04LiM02Li++ e + MO2LiCe Li++ e" + CeThird Electrode (electrode 3; cathode):Li++ e + MPO4 LiMPCE

[0247] In some embodiments, the first tank and the second tank comprise the same electrolyte (i.e., aqueous). In some embodiments, the second tank and the third tank comprise the same electrolyte (i.e., organic). In some embodiments, the electrolyte of the second can be changed between reaction 1 and reaction 2.

[0248] In some embodiments, referring to FIG. 3, the system comprises a two-chamber design. In some embodiments, a first chamber comprises a first tank (tank A) and a second tank (tank B). In some embodiments, a second chamber comprises a second tank (tank B) and a third tank (tank C). In some embodiments, the second tank of the first chamber comprises a second electrode (electrode 2a; an intermediate electrode) and the second tank of the second chamber comprises a second electrode (electrode 2b; a lithium-rich intermediate electrode). In some embodiments, for reaction 2, the second electrode (electrode 2a) in the first chamber is moved to the secondchamber (as electrode 2b) after reaction 1. In some embodiments, the electrolyte of the second tank can be changed between reaction 1 and reaction 2.

[0249] In some cases, the intermediate electrode can be non-reactive with non-lithium components in the aqueous source. The first chamber can have a one-chamber design. The first chamber comprises an anode, a de-lithiated cathode, and brine. In some embodiments, the de- lithiated cathode can be a coiled electrode. In some embodiments, the first chamber comprises an aqueous source comprising Li, a working electrode, and a counter electrode. The electrodes are water-stable electrodes that include but are not limited to LFP, LMO, LCO on Ti or carbon current collector. In some embodiments, the first chamber comprises water-stable slurry that include but are not limited to carbon coated LFP with conductive additive.

[0250] In some cases, the intermediate electrode can be reactive with non-lithium components in the aqueous source. The first chamber can have a two-chamber design. In this example, the first chamber comprises an anode, a de-lithiated cathode, brine, a membrane, an organic / polymer electrolyte. In some embodiments, the de-lithiated cathode can be a coiled electrode. In some embodiments, membrane is a lithium ion-selective membrane that physically separates the de- lithiated cathode and an organic / polymer electrolyte from the anode and brine. In some embodiments, the first chamber comprises two phases. In some embodiments, the first chamber comprises an aqueous source comprising Li with a counter electrode, a water-blocking membrane, an organic electrolyte, and a working electrode. The electrodes are water-unstable electrodes that include but are not limited to NMC, LFP, LMO, or LTO, on the metal current collector. In some embodiments, the first chamber comprises water-unstable electrodes or metal alloys that include but are not limited to graphite, Al, Mg, or Zn.

[0251] The second chamber can comprise a current collector foil and a Li+rich electrode as spiral rolls to produce a crude Li metal electrode. In some embodiments, the current collector foil comprises a current collector. In some embodiments, the Li+rich electrode comprises a current collector. In some embodiments, the current collector foil and the Li+rich electrode are physically separated by a separator. In some embodiments, the crude metal electrode can be treated by refining or post processes.

[0252] In some embodiments, the first chamber can be wound spiral or prismatic. In some embodiments, the first chamber can be a planar bath. In some embodiments, the membrane can be a separator between two liquid phases, or a polymer / gel that is directly coating the intermediate electrode. In some embodiments, the system can comprise a cylindrical cell . In some embodiments, the cylindrical cell can be a large steel can for the application of pressure. Insome embodiments, the cylindrical cell comprises a spring-loaded cake pan. In some embodiments, the cylindrical cell comprises a central mandrel to prevent roll collapse.

[0253] In some embodiments, the electrode can be further optionally treated by two-step refining processes. As a first step, pressure and heat can simultaneously be applied to the electrode during the refining step resulting in a dense and smooth electrodeposited lithium. In some embodiments, the pressure ranges from 0.5 to 10 MPa and the heat temperature ranges from 20 to 300 °C to modify the electrodeposited lithium morphology. As a second step, the electrodeposited Li is treated by rolling between two flat surfaces to create a mirror finish lithium surface.

[0254] In certain aspects, this disclosure provides a system for manufacturing a lithium metal electrode. The system can operate independently of the lithium source, maintaining a consistent output rate, quality, and location, regardless of the origin of the lithium used. A variety of lithium sources can be used (having varied compositions, impurities, etc.), because the intermediate electrode can selectively extract lithium from lithium sources. The system can not require constant operation to maintain a high temperature; it can be capable of functioning efficiently even under cold conditions. Thus, renewable energy sources that provide sporadic or inconsistent levels of energy and power could be used to lithiate and / or delithiate the intermediate electrode.

[0255] In some cases, the system comprises a first widget and a second widget. The first widget can be configured to contact an aqueous source comprising lithium with an intermediate electrode, thereby transferring the lithium to the intermediate electrode to form a lithium-rich intermediate electrode. The second widget can be configured to transfer the lithium from the lithium-rich intermediate electrode to a current collector substrate to form the lithium metal electrode. In some cases, the first widget and the second widget can be physically separate devices. In some cases, the first widget and the second widget can be combined to make one device. In some cases, the system comprises a renewable energy source configured to provide electrical power to transfer the lithium. In some cases, the renewable energy source comprises solar energy, wind energy, marine energy, geothermal energy, or any combination thereof.

[0256] In some embodiments, the aqueous source comprising lithium is brine. In some embodiments, the aqueous source comprising lithium further comprises Na+, K+, Mg2+, Ca2+, B(OH)4, Fe2+, Fe3+, Mn2+, MnO , MnO4, Cl’, SO42’, NH3, NH4+, NH40H, NO2, HN02, NO3’, an alkali metal ions, an alkali earth metal ions, or any combination thereof. In some embodiments, the aqueous source comprising lithium comprises a geological resource. In some embodiments, the aqueous source comprising lithium can be pretreated to remove Na+, K+, Mg2+,Ca2+, B(OH)4, Fe2+, Fe3+, Mn2+, MnO42, MnO4, Cl; SO42NH3, NH4+, NH4OH, NO2, HNO2, NO3an alkali metal ions, an alkali earth metal ions, or any combination thereof.

[0257] In some embodiments, the first widget comprises a counter electrode. In the first widget, the intermediate electrode can be connected with the counter electrode in a circuit, using the aqueous source comprising lithium as an electrolyte.

[0258] In some embodiments, the intermediate electrode comprises iron phosphate (FePO4), manganese oxide (MnCh), or nickel manganese cobalt oxide (NixMnyCoi-x-yCh). In some embodiments, the intermediate electrode comprises iron phosphate (FePO4). In some embodiments, the intermediate electrode comprises manganese oxide (MnCh). In some embodiments, the intermediate electrode comprises nickel manganese cobalt oxide (NixMnyCoi- x-yCh).

[0259] In some embodiments, the intermediate electrode comprises a metal current collector or a carbon current collector. In some embodiments, the intermediate electrode comprises the metal current collector. In some embodiments, the metal current collector comprises copper (Cu), titanium (Ti), aluminum (Al), magnesium (Mg), zinc (Zn), tin (Sn), vanadium oxide (V2O5), or any metal that is capable of forming an alloy with lithium. In some embodiments, the metal current collector comprises titanium (Ti). In some embodiments, the metal current collector comprises aluminum (Al). In some embodiments, the metal current collector comprises magnesium (Mg). In some embodiments, the metal current collector comprises zinc (Zn). In some embodiments, the metal current collector comprises tin (Sn). In some embodiments, the metal current collector comprises vanadium oxide (V2O5). In some embodiments, the metal current collector comprises any metal that is capable of forming an alloy with lithium.

[0260] In some embodiments, the intermediate electrode comprises the carbon current collector. In some embodiments, the carbon current collector comprises graphite. In some embodiments, the intermediate electrode comprises an electrically conductive slurry comprising an electrically conductive additive. In some embodiments, the intermediate electrode is obtained from recycled lithium-ion battery materials. In some embodiments, the intermediate electrode is obtained from black mass produced from shredding lithium-ion battery materials.

[0261] In some embodiments, the first widget can be configured to transfer the lithium from the aqueous source to the intermediate electrode by intercalating the lithium in the intermediate electrode to form the lithium-rich intermediate electrode.-n-

[0262] Before contacting the aqueous source comprising lithium, the intermediate electrode can be substantially free of lithium or can be in a de-lithiated state. In some embodiments, the lithium-rich intermediate electrode operates as a lithium ink.

[0263] In some embodiments, the first widget operates at temperatures up to about 95°C. In some embodiments, the first widget operates at ambient temperature or room temperature. In some embodiments, the first widget operates at temperature of 15°C, 20°C, 25°C, 30°C, 35°C, 40°C, 45°C, 50°C, 55°C, 60°C, 65°C, 70°C, 75°C, 80°C, 85°C, 90°C, or 95°C. In some embodiments, the first widget operates at temperature of about 15°C, about 20°C, about 25°C, about 30°C, about 35°C, about 40°C, about 45°C, about 50°C, about 55°C, about 60°C, about 65°C, about 70°C, about 75°C, about 80°C, about 85°C, about 90°C, or about 95°C, including all values and sub ranges in between. In some embodiments, the first widget operates at temperature of at least 15°C, at least 20°C, at least 25°C, at least 30°C, at least 35°C, at least 40°C, at least 45°C, at least 50°C, at least 55°C, at least 60°C, at least 65°C, at least 70°C, at least 75°C, at least 80°C, at least 85°C, at least 90°C, or at least 95°C. In some embodiments, the first widget operates at temperature of at most 15°C, at most 20°C, at most 25°C, at most 30°C, at most 35°C, at most 40°C, at most 45°C, at most 50°C, at most 55°C, at most 60°C, at most 65°C, at most 70°C, at most 75°C, at most 80°C, at most 85°C, at most 90°C, at most 95°C, or at most 98°C.

[0264] In some embodiments, the second widget can be configured to apply an electric potential across the lithium-rich intermediate electrode and the current collector substrate.

[0265] In some embodiments, the lithium-rich intermediate electrode comprises lithium iron phosphate (LiFePCU, LFP), lithium manganese oxide (LiMn2O4 spinel, or Li2MnO3-based lithium-rich layered materials, LMR-NMC), lithium nickel manganese cobalt oxide (LiNiMnCoCh or NMC), lithium manganate (Li2MnO4, LMO), LiCe, LixMgy, LixAly, LixSiy, or a combination thereof. In some embodiments, the lithium-rich intermediate electrode comprises lithium iron phosphate (LiFePC , LFP). In some embodiments, the lithium-rich intermediate electrode comprises lithium manganese oxide (LiMn2O4 spinel, or Li2MnO3-based lithium-rich layered materials, LMR-NMC). In some embodiments, the lithium-rich intermediate electrode comprises lithium nickel manganese cobalt oxide (LiNiMnCoCh or NMC).

[0266] In some embodiments, the second widget can be configured to transfer the lithium from the lithium-rich intermediate electrode to the current collector substrate by delithiating the lithium-rich intermediate electrode. In some embodiments, the intercalating and the delithiating are reversible. In some embodiments, the transferring the lithium to the current collector substrate comprises coating or printing the (lithium) ink on the current collector substrate. Insome embodiments, printing comprises plating lithium from lithium-rich electrode to a current collector substrate.

[0267] In some embodiments, the current collector substrate comprises copper, copper alloy, aluminum, aluminum alloy, titanium, titanium alloy, nickel, nickel alloy, stainless steel, carbonaceous material, or any combination thereof. In some embodiments, the current collector substrate comprises Cu. In some embodiments, the current collector substrate comprises Cu-Ni, Cu-Ti, Cu-Zn, Cu-Al, Cu-Sn, Ni-CO, Al -Mg, Fe-Cr-Ni, or any combination thereof. In some embodiments, the current collector substrate comprises Al. In some embodiments, the current collector substrate comprises Ni. In some embodiments, the current collector substrate comprises Ti. In some embodiments, the current collector substrate comprises stainless steel. In some embodiments, the current collector substrate comprises carbonaceous material. In some embodiments, a current collector substrate comprises copper, stainless steel, aluminum, nickel, titanium, sintered carbon, copper or stainless steel that is surface-treated with carbon, nickel, titanium or silver, and aluminum-cadmium alloys. In some embodiments, a current collector substrate comprises fine irregularities on surfaces thereof so as to enhance adhesive strength of the electrode current collector substrate to the electrode active material.

[0268] In some embodiments, a current collector substrate can comprise various forms including films, sheets, foils, nets, porous structures, foams, and non-woven fabrics. In some embodiments, a current collector substrate comprises carbon, carbon paper, carbon cloth or a metal or noble metal mesh or foil.

[0269] In some embodiments, an electrical connection to the lithium-rich intermediate electrode is made via copper, copper alloy, aluminum, aluminum alloy, titanium, titanium alloy, nickel, nickel alloy, stainless steel, carbonaceous material, or any combination thereof. In some embodiments, the lithium-rich intermediate electrode comprises copper, stainless steel, aluminum, nickel, titanium, sintered carbon, copper or stainless steel that is surface-treated with carbon, nickel, titanium or silver, and aluminum-cadmium alloys.

[0270] In some embodiments, the lithium-rich intermediate electrode can comprise various forms including films, sheets, foils, nets, porous structures, foams, and non-woven fabrics. In some embodiments, the lithium-rich intermediate electrode comprises carbon, carbon paper, carbon cloth or a metal or noble metal mesh or foil. The transferring of the lithium from the lithium-rich intermediate electrode to the current collector substrate comprises electrodeposition of the lithium as a layer of lithium metal on the current collector substrate.

[0271] In some embodiments, the lithium can be electrodeposited as a layer of lithium metal at least 1 micrometer (pm) thickness of a layer / min. In some embodiments, the lithium can be electrodeposited as a layer of lithium metal at 0.1 pm / min, 0.2 pm / min, 0.3 pm / min, 0.4 pm / min, 0.5 pm / min, 0.6 pm / min, 0.7 pm / min, 0.8 pm / min, 0.9 pm / min, 1 pm / min, 1.1 pm / min, 1.2 pm / min, 1.3 pm / min, 1.4 pm / min, 1.5 pm / min, 1.6 pm / min, 1.7 pm / min, 1.8 pm / min, 1.9 pm / min, 2 pm / min, 2.2 pm / min, 2.4 pm / min, 2.6 pm / min, 2.8 pm / min, 3 pm / min, 3.2 pm / min, 3.4 pm / min, 3.6 pm / min, 3.8 pm / min, 4 pm / min, 4.2 pm / min,4.4 pm / min, 4.6 pm / min, 4.8 pm / min, or 5 pm / min. In some embodiments, the lithium can be electrodeposited as a layer of lithium metal at about 0.1 pm / min, about 0.2 pm / min, about 0.3 pm / min, about 0.4 pm / min, about 0.5 pm / min, about 0.6 pm / min, about 0.7 pm / min, about 0.8 pm / min, about 0.9 pm / min, about 1 pm / min, about 1.1 pm / min, about 1.2 pm / min, about1.3 pm / min, about 1.4 pm / min, about 1.5 pm / min, about 1.6 pm / min, about 1.7 pm / min, about1.8 pm / min, about 1.9 pm / min, about 2 pm / min, about 2.2 pm / min, about 2.4 pm / min, about2.6 pm / min, about 2.8 pm / min, about 3 pm / min, about 3.2 pm / min, about 3.4 pm / min, about3.6 pm / min, about 3.8 pm / min, about 4 pm / min, about 4.2 pm / min, about 4.4 pm / min, about4.6 pm / min, about 4.8 pm / min, or about 5 pm / min, including all values and sub ranges in between. In some embodiments, the lithium can be electrodeposited as a layer of lithium metal at least 0.1 pm / min, at least 0.2 pm / min, at least 0.3 pm / min, at least 0.4 pm / min, at least0.5 pm / min, at least 0.6 pm / min, at least 0.7 pm / min, at least 0.8 pm / min, at least 0.9 pm / min, at least 1 pm / min, at least 1.1 pm / min, at least 1.2 pm / min, at least 1.3 pm / min, at least1.4 pm / min, at least 1.5 pm / min, at least 1.6 pm / min, at least 1.7 pm / min, at least 1.8 pm / min, at least 1.9 pm / min, at least 2 pm / min, at least 2.2 pm / min, at least 2.4 pm / min, at least2.6 pm / min, at least 2.8 pm / min, at least 3 pm / min, at least 3.2 pm / min, at least 3.4 pm / min, at least 3.6 pm / min, at least 3.8 pm / min, at least 4 pm / min, at least 4.2 pm / min, at least4.4 pm / min, at least 4.6 pm / min, at least 4.8 pm / min, or at least 5 pm / min. In some embodiments, the lithium can be electrodeposited as a layer of lithium metal at most 0.1 pm / min, at most 0.2 pm / min, at most 0.3 pm / min, at most 0.4 pm / min, at most 0.5 pm / min, at most0.6 pm / min, at most 0.7 pm / min, at most 0.8 pm / min, at most 0.9 pm / min, at most 1 pm / min, at most 1.1 pm / min, at most 1.2 pm / min, at most 1.3 pm / min, at most 1.4 pm / min, at most1.5 pm / min, at most 1.6 pm / min, at most 1.7 pm / min, at most 1.8 pm / min, at most 1.9 pm / min, at most 2 pm / min, at most 2.2 pm / min, at most 2.4 pm / min, at most 2.6 pm / min, at most2.8 .m / min, at most 3 .m / min, at most 3.2 .m / min, at most 3.4 .m / min, at most 3.6 .m / min, at most 3.8 .m / min, at most 4 .m / min, at most 4.2 .m / min, at most 4.4 .m / min, at most 4.6 .m / min, at most 4.8 .m / min, or at most 5 .m / min.

[0272] In some embodiments, the electrodepositing comprises coating or printing the electrode ink on the current collector substrate.

[0273] In some embodiments, the second widget operates at a temperature of about 10°C to about 150°C. In some embodiments, the second widget operates at a temperature of 5°C, 10°C, 20°C, 30°C, 40°C, 50°C, 60°C, 70°C, 80°C, 90°C, 100°C, 110°C, 120°C, 130°C, 140°C, 150°C, 160°C, 170°C, 180°C, 190°C, or 200°C. In some embodiments, the second widget operates at a temperature of about 5°C, about 10°C, about 20°C, about 30°C, about 40°C, about 50°C, about 60°C, about 70°C, about 80°C, about 90°C, about 100°C, about 110°C, about 120°C, about 130°C, about 140°C, about 150°C, about 160°C, about 170°C, about 180°C, about 190°C, or about 200°C, including all values and sub ranges in between. In some embodiments, the second widget operates at a temperature of at least 5°C, at least 10°C, at least 20°C, at least 30°C, at least 40°C, at least 50°C, at least 60°C, at least 70°C, at least 80°C, at least 90°C, at least 100°C, at least 110°C, at least 120°C, at least 130°C, at least 140°C, at least 150°C, at least 160°C, at least 170°C, at least 180°C, at least 190°C, or at least 200°C. In some embodiments, the second widget operates at a temperature of at most 5°C, at most 10°C, at most 20°C, at most 30°C, at most 40°C, at most 50°C, at most 60°C, at most 70°C, at most 80°C, at most 90°C, at most 100°C, at most 110°C, at most 120°C, at most 130°C, at most 140°C, at most 150°C, at most 160°C, at most 170°C, at most 180°C, at most 190°C, or at most 200°C.

[0274] In some embodiments, the second widget operates at a pressure of about 0.05 MPa to about 15 MPa. In some embodiments, the second widget operates at a pressure of 0.01 MPa, 0.05 MPa, 0.1 MPa, 0.2 MPa, 0.3 MPa, 0.4 MPa, 0.5 MPa, 0.6 MPa, 0.7 MPa, 0.8 MPa, 0.9 MPa, 1 MPa, 1.5 MPa, 2 MPa, 2.5 MPa, 3 MPa, 3.5 MPa, 4 MPa, 4.5 MPa, 5 MPa, 5.5 MPa, 6 MPa, 6.5 MPa, 7 MPa, 7.5 MPa, 8 MPa, 8.5 MPa, 9 MPa, 9.5 MPa, 10 MPa, 10.5 MPa, 11 MPa, 11.5 MPa, 12 MPa, 12.5 MPa, 13 MPa, 13.5 MPa, 14 MPa, 14.5 MPa, 15 MPa, 15.5 MPa, 16 MPa, 16.5 MPa, 17 MPa, 17.5 MPa, or 18 MPa. In some embodiments, the second widget operates at a pressure of about 0.01 MPa, about 0.05 MPa, about 0.1 MPa, about 0.2 MPa, about 0.3 MPa, about 0.4 MPa, about 0.5 MPa, about 0.6 MPa, about 0.7 MPa, about 0.8 MPa, about 0.9 MPa, about 1 MPa, about 1.5 MPa, about 2 MPa, about 2.5 MPa, about 3 MPa, about 3.5 MPa, about 4 MPa, about 4.5 MPa, about 5 MPa, about 5.5 MPa, about 6 MPa, about 6.5 MPa, about 7 MPa, about 7.5 MPa, about 8 MPa, about 8.5 MPa, about 9 MPa, about 9.5 MPa, about 10 MPa, about10.5 MPa, about 11 MPa, about 11.5 MPa, about 12 MPa, about 12.5 MPa, about 13 MPa, about13.5 MPa, about 14 MPa, about 14.5 MPa, about 15 MPa, about 15.5 MPa, about 16 MPa, about16.5 MPa, about 17 MPa, about 17.5 MPa, or about 18 MPa, including all values and sub ranges in between. In some embodiments, the second widget operates at a pressure of at least 0.01 MPa, at least 0.05 MPa, at least 0.1 MPa, at least 0.2 MPa, at least 0.3 MPa, at least 0.4 MPa, at least 0.5 MPa, at least 0.6 MPa, at least 0.7 MPa, at least 0.8 MPa, at least 0.9 MPa, at least 1 MPa, at least 1.5 MPa, at least 2 MPa, at least 2.5 MPa, at least 3 MPa, at least 3.5 MPa, at least 4 MPa, at least 4.5 MPa, at least 5 MPa, at least 5.5 MPa, at least 6 MPa, at least 6.5 MPa, at least 7 MPa, at least 7.5 MPa, at least 8 MPa, at least 8.5 MPa, at least 9 MPa, at least 9.5 MPa, at least 10 MPa, at least 10.5 MPa, at least 11 MPa, at least 11.5 MPa, at least 12 MPa, at least 12.5 MPa, at least 13 MPa, at least 13.5 MPa, at least 14 MPa, at least 14.5 MPa, at least 15 MPa, at least 15.5 MPa, at least 16 MPa, at least 16.5 MPa, at least 17 MPa, at least 17.5 MPa, or at least 18 MPa. In some embodiments, the second widget operates at a pressure of at most 0.01 MPa, at most 0.05 MPa, at most 0.1 MPa, at most 0.2 MPa, at most 0.3 MPa, at most 0.4 MPa, at most 0.5 MPa, at most 0.6 MPa, at most 0.7 MPa, at most 0.8 MPa, at most 0.9 MPa, at most 1 MPa, at most 1.5 MPa, at most 2 MPa, at most 2.5 MPa, at most 3 MPa, at most 3.5 MPa, at most 4 MPa, at most 4.5 MPa, at most 5 MPa, at most 5.5 MPa, at most 6 MPa, at most 6.5 MPa, at most 7 MPa, at most 7.5 MPa, at most 8 MPa, at most 8.5 MPa, at most 9 MPa, at most 9.5 MPa, at most 10 MPa, at most 10.5 MPa, at most 11 MPa, at most 11.5 MPa, at most 12 MPa, at most12.5 MPa, at most 13 MPa, at most 13.5 MPa, at most 14 MPa, at most 14.5 MPa, at most 15 MPa, at most 15.5 MPa, at most 16 MPa, at most 16.5 MPa, at most 17 MPa, at most 17.5 MPa, or at most 18 MPa.

[0275] In some embodiments, the second widget operates at about 0.1 mA / cm2to about 30 mA / cm2. In some embodiments, the second widget operates at 0.05 mA / cm2, 0.1 mA / cm2, 0.5 mA / cm2, 1 mA / cm2, 2 mA / cm2, 3 mA / cm2, 4 mA / cm2, 5 mA / cm2, 6 mA / cm2, 7 mA / cm2, 8 mA / cm2, 9 mA / cm2, 10 mA / cm2, 12 mA / cm2, 14 mA / cm2, 16 mA / cm2, 18 mA / cm2, 20 mA / cm2, 22 mA / cm2, 24 mA / cm2, 26 mA / cm2, 28 mA / cm2, 30 mA / cm2, 32 mA / cm2, 34 mA / cm2, 36 mA / cm2, 38 mA / cm2, or 40 mA / cm2. In some embodiments, the second widget operates at about 0.05 mA / cm2, about 0.1 mA / cm2, about 0.5 mA / cm2, about 1 mA / cm2, about 2 mA / cm2, about 3 mA / cm2, about 4 mA / cm2, about 5 mA / cm2, about 6 mA / cm2, about 7 mA / cm2, about 8 mA / cm2, about 9 mA / cm2, about 10 mA / cm2, about 12 mA / cm2, about 14 mA / cm2, about 16 mA / cm2, about 18 mA / cm2, about 20 mA / cm2, about 22 mA / cm2, about 24 mA / cm2, about 26 mA / cm2, about 28 mA / cm2, about 30 mA / cm2, about 32 mA / cm2, about 34 mA / cm2, about 36 mA / cm2,about 38 mA / cm2, or about 40 mA / cm2, including all values and sub ranges in between. In some embodiments, the second widget operates at least 0.05 mA / cm2, at least 0.1 mA / cm2, at least 0.5 mA / cm2, at least 1 mA / cm2, at least 2 mA / cm2, at least 3 mA / cm2, at least 4 mA / cm2, at least 5 mA / cm2, at least 6 mA / cm2, at least 7 mA / cm2, at least 8 mA / cm2, at least 9 mA / cm2, at least 10 mA / cm2, at least 12 mA / cm2, at least 14 mA / cm2, at least 16 mA / cm2, at least 18 mA / cm2, at least 20 mA / cm2, at least 22 mA / cm2, at least 24 mA / cm2, at least 26 mA / cm2, at least 28 mA / cm2, at least 30 mA / cm2, at least 32 mA / cm2, at least 34 mA / cm2, at least 36 mA / cm2, at least 38 mA / cm2, or at least 40 mA / cm2. In some embodiments, the second widget operates at most 0.05 mA / cm2, at most 0.1 mA / cm2, at most 0.5 mA / cm2, at most 1 mA / cm2, at most 2 mA / cm2, at most 3 mA / cm2, at most 4 mA / cm2, at most 5 mA / cm2, at most 6 mA / cm2, at most 7 mA / cm2, at most 8 mA / cm2, at most 9 mA / cm2, at most 10 mA / cm2, at most 12 mA / cm2, at most 14 mA / cm2, at most 16 mA / cm2, at most 18 mA / cm2, at most 20 mA / cm2, at most 22 mA / cm2, at most 24 mA / cm2, at most 26 mA / cm2, at most 28 mA / cm2, at most 30 mA / cm2, at most 32 mA / cm2, at most 34 mA / cm2, at most 36 mA / cm2, at most 38 mA / cm2, or 4 at most 40 mA / cm2.

[0276] In some embodiments, the second widget comprises an electrolyte. The electrolyte includes, but is not limited to, (a) 1,3-dioxolane (DOL): 1,2-dimethoxy ethane (DME), 1 M lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), 1% LiNCL, (b) 2EC (ethylene carbonate): 3 EMC (ethyl methyl carbonate), 1 M LiTFSI, (c) tetraethylene glycol dimethyl ether (G4), 1 M LiNCE, (d) diethylene glycol dimethyl ether (G2), 1 M LiNCh, (e) G4, 1 M LiTFSI, or (f) bis(2-fluoroethoxy)methane (F2DEM), 1,75 M LiTFSI. The electrolyte can comprise solid electrolytes. Employing a solid electrolyte could significantly mitigate electrolyte loss, thereby leading to considerable savings in the costs associated with electrolyte replacement.

[0277] In some embodiments, the electrolyte can be evaporated or boiled to recover the electrolyte. In some embodiments, a boiling point of the electrolyte ranges from about 70°C to about 350°C. In some embodiments, a boiling point of the electrolyte is 70°C, 90°C, 110°C, 130°C, 150°C, 170°C, 190°C, 200°C, 210°C, 230°C, 250°C, 270°C, 290°C, 310°C, 330°C, or 350°C. In some embodiments, a boiling point of the electrolyte is about 70°C, about 90°C, about 110°C, about 130°C, about 150°C, about 170°C, about 190°C, about 200°C, about 210°C, about 230°C, about 250°C, about 270°C, about 290°C, about 310°C, about 330°C, or about 350°C, including all values and sub ranges in between. In some embodiments, a boiling point of the electrolyte is at least 70°C, at least 90°C, at least 110°C, at least 130°C, at least 150°C, at least 170°C, at least 190°C, at least 200°C, at least 210°C, at least 230°C, at least 250°C, at least 270°C, at least 290°C, at least 310°C, at least 330°C, or at least 350°C. In some embodiments, aboiling point of the electrolyte is at most 110°C, at most 130°C, at most 150°C, at most 170°C, at most 190°C, at most 200°C, at most 210°C, at most 230°C, at most 250°C, at most 270°C, at most 290°C, at most 310°C, at most 330°C, or at most 350°C. In some a boiling point of the electrolyte can be 275°C. In some a boiling point of the electrolyte can be 162°C. The electrolyte can be non-volatile. In some embodiments, the electrolyte can not evaporate during the operation of the second widget.

[0278] In some embodiments, the second widget can be configured to provide a separator between the lithium rich intermediate electrode and the current collector substrate. In some embodiments, the second widget comprises two input rolls of lithium supply, two input rolls of separator to produce a two-sided lithium printing. In some embodiments, the separator comprises a lithium ion-selective membrane permitting lithium ions to selectively flow through. The lithium ion-selective membrane comprises a single layer or multiple layers. In some embodiments, the lithium ion-selective membrane comprises a single layer. In some embodiments, the lithium ion-selective membrane comprises multiple layers.

[0279] In some embodiments, the lithium ion-selective membrane comprises glass fiber, polyester, polyethylene, polypropylene, polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), and a combination thereof. In some embodiments, the lithium ion-selective membrane comprises hydrophobic polymers. In some embodiments, the lithium ion-selective membrane comprises lithium-ion conductive channels.

[0280] In some embodiments, a columbic efficiency of the system ranges from about 60% to about 100%. In some embodiments, a stripping efficiency of the second widget is 60%, 65%, 70%, 75%, 80%, 85%, 88%, 90%, 92%, 94%, 96%, 98%, or 100%. In some embodiments, a columbic efficiency of the system is about 60%, about 65%, about 70%, about 75%, about 80%, about 85%, about 88%, about 90%, about 92%, about 94%, about 96%, about 98%, or about 100%, including all values and sub ranges in between. In some embodiments, a columbic efficiency of the system is at least 60%, at least 65%, at least 70%, at least 75%, at least 80%, at least 85%, at least 88%, at least 90%, at least 92%, at least 94%, at least 96%, at least 98%, or at least 100%. In some embodiments, a columbic efficiency of the system is at most 70%, at most 75%, at most 80%, at most 85%, at most 88%, at most 90%, at most 92%, at most 94%, at most 96%, at most 98%, or at most 100%. In some embodiments, a columbic efficiency of the system ranges from about 80% to about 100%.

[0281] In some embodiments, a deposition efficiency of the second widget ranges from about 90% to about 100%. In some embodiments, a deposition efficiency of the second widget is 90%,91%, 92%, 93%, 94%, 95%, 96%, 97%, 98%, 99%, or 100%. In some embodiments, a deposition efficiency of the second widget is about 90%, about 91%, about 92%, about 93%, about 94%, about 95%, about 96%, about 97%, about 98%, about 99%, or about 100%, including all values and sub ranges in between. In some embodiments, a deposition efficiency of the second widget is at least 90%, at least 91%, at least 92%, at least 93%, at least 94%, at least 95%, at least 96%, at least 97%, at least 98%, at least 99%, or at least 100%. In some embodiments, a stripping efficiency of the second widget is at most 92%, at most 93%, at most 94%, at most 95%, at most 96%, at most 97%, at most 98%, at most 99%, or at most 100%. In some embodiments, a deposition efficiency of the second widget ranges from about 95%. In some embodiments, a deposition efficiency of the second widget ranges from about 98%. In some embodiments, a deposition efficiency of the second widget ranges from about 99%. In some embodiments, a deposition efficiency of the second widget ranges from about 97%. In some embodiments, a deposition efficiency of the second widget ranges from about 96%.

[0282] In some embodiments, the second widget can be configured to produce a two-sided lithium metal electrode. In some embodiments, the second widget can be configured to produce an all-sided lithium metal electrode. In some embodiments, the produced lithium metal electrode is a battery -ready electrode.

[0283] The surface roughness of the lithium metal electrode can be determined by various tools including, but not limited to, surface profilometry, Atomic Force Microscopy (AFM), Scanning Electron Microscopy (SEM), White Light Interferometry, or Laser Scanning Confocal Microscopy (LSCM) (FIG. 9). In some embodiments, a surface roughness of the lithium metal electrode is less than about 3.0 micrometer (pm). In some embodiments, a surface roughness of the lithium metal electrode is less than about 1.0 pm. In some embodiments, a surface roughness of the lithium metal electrode is 0.02 pm, 0.04 pm, 0.06 pm, 0.08 pm, 0.1 pm, 0.15 pm, 0.2 pm, 0.25 pm, 0.3 pm, 0.35 pm, 0.4 pm, 0.45 pm, 0.5 pm, 0.55 pm, 0.6 pm, 0.65, 0.7 pm, 0.75 pm, 0.8 pm, 0.85 pm, 0.9 pm, 0.95 pm, 1.0 pm, 1.2 pm, 1.4 pm, 1.6 pm, 1.8 pm, 2.0 pm, 2.2 pm, 2.4 pm, 2.6 pm, 2.8 pm, 3.0 pm, 3.2 pm, 3.4 pm, 3.6 pm, 3.8 pm, or 4.0 pm. In some embodiments, a surface roughness of the lithium metal electrode is about 0.02 pm, about 0.04 pm, about 0.06 pm, about 0.08 pm, about 0.1 pm, about 0.15 pm, about 0.2 pm, about 0.25 pm, about 0.3 pm, about 0.35 pm, about 0.4 pm, about 0.45 pm, about 0.5 pm, about 0.55 pm, about 0.6 pm, about 0.65, about 0.7 pm, about 0.75 pm, about 0.8 pm, about 0.85 pm, about 0.9 pm, about 0.95 pm, about 1.0 pm, about 1.2 pm, about 1.4 pm, about 1.6 pm, about 1.8 pm, about2.0 pm, about 2.2 pin, about 2.4 pm, about 2.6 pm, about 2.8 pm, about 3.0 pm, about 3.2 pm, about 3.4 pm, about 3.6 pm, about 3.8 pm, or about 4.0 pm, including all values and sub ranges in between. In some embodiments, a surface roughness of the lithium metal electrode is at most 0.02 pm, at most 0.04 pm, at most 0.06 pm, at most 0.08 pm, at most 0.1 pm, at most 0.15 pm, at most 0.2 pm, at most 0.25 pm, at most 0.3 pm, at most 0.35 pm, at most 0.4 pm, at most 0.45 pm, at most 0.5 pm, at most 0.55 pm, at most 0.6 pm, at most 0.65, at most 0.7 pm, at most 0.75 pm, at most 0.8 pm, at most 0.85 pm, at most 0.9 pm, at most 0.95 pm, at most 1.0 pm, at most1.2 pm, at most 1.4 pm, at most 1.6 pm, at most 1.8 pm, at most 2.0 pm, at most 2.2 pm, at most 2.4 pm, at most 2.6 pm, at most 2.8 pm, at most 3.0 pm, at most 3.2 pm, at most 3.4 pm, at most 3.6 pm, at most 3.8 pm, or at most 4.0 pm.

[0284] The measurements of surface roughness are shown in FIG. 10. In some embodiments, the lithium metal electrode has a 0.5 pm, 1 pm, 1.1 pm, 1.2 pm, 1.3 pm, 1.4 pm, 1.5 pm, 1.6 pm, 1.7 pm, 1.8 pm, 1.9 pm, 2 pm, 2.1 pm, 2.2 pm, 2.3 pm, 2.4 pm, 2.5 pm, 3 pm, 3.5 pm, 4 pm, 4.5 pm, 5 pm, 5.5 pm, 6 pm, 6.5 pm, 7 pm, 7.5 pm, 8 pm, 8.5 pm, 9 pm, 9.5 pm, or 10 pm defect (Sp). In some embodiments, the lithium metal electrode has an about 0.5 pm, about 0.6 pm, about 0.7 pm, about 0.8 pm, about 0.9 pm, about 1 pm, about 1.1 pm, about 1.2 pm, about1.3 pm, about 1.4 pm, about 1.5 pm, about 1.6 pm, about 1.7 pm, about 1.8 pm, about 1.9 pm, about 2 pm, about 2.1 pm, about 2.2 pm, about 2.3 pm, about 2.4 pm, about 2.5 pm, about 3 pm, about 3.5 pm, about 4 pm, about 4.5 pm, about 5 pm, about 5.5 pm, about 6 pm, about 6.5 pm, about 7 pm, about 7.5 pm, about 8 pm, about 8.5 pm, about 9 pm, about 9.5 pm, or about 10 pm defect (Sp). In some embodiments, the lithium metal electrode has an at least 0.5 pm, at least 0.6 pm, at least 0.7 pm, at least 0.8 pm, at least 0.9 pm, at least 1 pm, at least 1.1 pm, at least 1.2 pm, at least 1.3 pm, at least 1.4 pm, at least 1.5 pm, at least 1.6 pm, at least 1.7 pm, at least 1.8 pm, at least 1.9 pm, at least 2 pm, at least 2.1 pm, at least 2.2 pm, at least 2.3 pm, at least 2.4 pm, at least 2.5 pm, at least 3 pm, at least 3.5 pm, at least 4 pm, at least 4.5 pm, at least5 pm, at least 5.5 pm, at least 6 pm, at least 6.5 pm, at least 7 pm, at least 7.5 pm, at least 8 pm, at least 8.5 pm, at least 9 pm, at least 9.5 pm, or at least 10 pm defect (Sp). In some embodiments, the lithium metal electrode has an at most 0.5 pm, at most 0.6 pm, at most 0.7 pm, at most 0.8 pm, at most 0.9 pm, at most 1 pm, at most 1.1 pm, at most 1.2 pm, at most 1.3 pm, at most 1.4 pm, at most 1.5 pm, at most 1.6 pm, at most 1.7 pm, at most 1.8 pm, at most 1.9 pm, at most 2 pm, at most 2.1 pm, at most 2.2 pm, at most 2.3 pm, at most 2.4 pm, at most 2.5 pm,at most 3 m, at most 3.5 pm, at most 4 pm, at most 4.5 pm, at most 5 pm, at most 5.5 pm, at most 6 pm, at most 6.5 pm, at most 7 pm, at most 7.5 pm, at most 8 pm, at most 8.5 pm, at most 9 pm, at most 9.5 pm, or 10 pm defect (Sp).

[0285] The measurements of surface roughness are shown in FIG. 10. In some embodiments, the lithium metal electrode has an average roughness of at most 1.6 microns (pm) (Sa). In some embodiments, the lithium metal electrode has an average roughness of 0.1 microns (pm), 0.12 pm, 0.14 pm, 0.16 pm, 0.18 pm, 0.2 pm, 0.22 pm, 0.24 pm, 0.26 pm, 0.28 pm, 0.3 pm, 0.32 pm, 0.34 pm, 0.36 pm, 0.38 pm, 0.4 pm, 0.45 pm, 0.5 pm, 0.55 pm, 0.6 pm, 0.65 pm, 0.7 pm, 0.75 pm, 0.8 pm, 0.85 pm, 0.9 pm, 0.95 pm, 1 pm, 1.2 pm, 1.4 pm, 1.6 pm, 1.8 pm, or 2 pm (Sa). In some embodiments, the lithium metal electrode has an average roughness of about 0.1 pm, about 0.12 pm, about 0.14 pm, about 0.16 pm, about 0.18 pm, about 0.2 pm, about 0.22 pm, about 0.24 pm, about 0.26 pm, about 0.28 pm, about 0.3 pm, about 0.32 pm, about 0.34 pm, about 0.36 pm, about 0.38 pm, about 0.4 pm, about 0.45 pm, about 0.5 pm, about 0.55 pm, about 0.6 pm, about 0.65 pm, about 0.7 pm, about 0.75 pm, about 0.8 pm, about 0.85 pm, about 0.9 pm, about 0.95 pm, about 1 pm, about 1.2 pm, about 1.4 pm, about 1.6 pm, about 1.8 pm, or about 2 pm (Sa). In some embodiments, the lithium metal electrode has an average roughness of at least 0.1 pm, at least 0.12 pm, at least 0.14 pm, at least 0.16 pm, at least 0.18 pm, at least 0.2 pm, at least 0.22 pm, at least 0.24 pm, at least 0.26 pm, at least 0.28 pm, at least 0.3 pm, at least 0.32 pm, at least 0.34 pm, at least 0.36 pm, at least 0.38 pm, at least 0.4 pm, at least 0.45 pm, at least 0.5 pm, at least 0.55 pm, at least 0.6 pm, at least 0.65 pm, at least 0.7 pm, at least 0.75 pm, at least 0.8 pm, at least 0.85 pm, at least 0.9 pm, at least 0.95 pm, at least 1 pm, at least 1.2 pm, at least 1.4 pm, at least 1.6 pm, at least 1.8 pm, or at least 2 pm (Sa). In some embodiments, the lithium metal electrode has an average roughness of at most 0.1 pm, at most 0.12 pm, at most 0.14 pm, at most 0.16 pm, at most 0.18 pm, at most 0.2 pm, at most 0.22 pm, at most 0.24 pm, at most 0.26 pm, at most 0.28 pm, at most 0.3 pm, at most 0.32 pm, at most 0.34 pm, at most 0.36 pm, at most 0.38 pm, at most 0.4 pm, at most 0.45 pm, at most 0.5 pm, at most 0.55 pm, at most 0.6 pm, at most 0.65 pm, at most 0.7 pm, at most 0.75 pm, at most 0.8 pm, at most 0.85 pm, at most 0.9 pm, at most 0.95 pm, at most 1 pm, at most 1.2 pm, at most 1.4 pm, at most 1.6 pm, at most 1.8 pm, or at most 2 pm (Sa).

[0286] A nodule size of the lithium metal electrode can be highly tunable depending on deposition condition. The measurements of nodule size are shown in FIG. 11. In someembodiments, a nodule size of the lithium metal electrode is 10 m to 15 pm in diameter. In some embodiments, a nodule size of the lithium metal electrode is 1 pm to 40 pm in diameter. In some embodiments, a nodule size of the lithium metal electrode is 1 pm to 60 pm in diameter. In some embodiments, a nodule size of the lithium metal layer on the current collector substrate is 1 pm, 5 pm, 10 pm, 11 pm, 12 pm, 13 pm, 14 pm, 15 pm, 16 pm, 17 pm, 18 pm, 19 pm, 20 pm, 25 pm, 30 pm, 35 pm, 40 pm, 45 pm, 50 pm, 55 pm, or 60 pm in diameter. In some embodiments, a nodule size of the lithium metal electrode is about 1 pm, about 5 pm, about 10 pm, about 11 pm, about 12 pm, about 13 pm, about 14 pm, about 15 pm, about 16 pm, about 17 pm, about 18 pm, about 19 pm, about 20 pm, about 25 pm, about 30 pm, about 35 pm, about 40 pm, about 45 pm, about 50 pm, about 55 pm, or about 60 pm in diameter. In some embodiments, a nodule size of the lithium metal electrode is at least 1 pm, at least 5 pm, at least 10 pm, at least 11 pm, at least 12 pm, at least 13 pm, at least 14 pm, at least 15 pm, at least 16 pm, at least 17 pm, at least 18 pm, at least 19 pm, at least 20 pm, at least 25 pm, at least 30 pm, at least 35 pm, at least 40 pm, at least 45 pm, at least 50 pm, at least 55 pm, or at least 60 pm in diameter. In some embodiments, a nodule size of the lithium metal electrode is at most 1 pm, at most 5 pm, at most 10 pm, at most 11 pm, at most 12 pm, at most 13 pm, at most 14 pm, at most 15 pm, at most 16 pm, at most 17 pm, at most 18 pm, at most 19 pm, at most 20 pm, at most 25 pm, at most 30 pm, at most 35 pm, at most 40 pm, at most 45 pm, at most 50 pm, at most 55 pm, or at most 60 pm in diameter.

[0287] The purity of the lithium metal electrode can be determined by several analytical techniques, including but not limited to Inductively Coupled Plasma Mass Spectrometry (ICP- MS), Atomic Absorption Spectroscopy (AAS), X-Ray Fluorescence (XRF), or Inductively Coupled Plasma Optical Emission Spectroscopy (ICP-OES). In some embodiments, a purity of the produced lithium metal electrode is higher than about 98%. In some embodiments, a purity of the produced lithium metal electrode is higher than about 99.9%. In some embodiments, a purity of the produced lithium metal electrode is 90%, 91%, 92%, 93%, 94%, 95%, 96%, 97%, 97.5%, 98%, 98.2%, 98.4%, 98.6%, 98.8%, 99%, 99.1%, 99.2%, 99.3%, 99.4%, 99.5%, 99.6%, 99.7%, 99.8%, 99.9%, 99.92%, 99.94%, 99.96%, 99.98%, or 100%. In some embodiments, a purity of the produced lithium metal electrode is about 90%, about 91%, about 92%, about 93%, about 94%, about 95%, about 96%, about 97%, about 97.5%, about 98%, about 98.2%, about 98.4%, about 98.6%, about 98.8%, about 99%, about 99.1%, about 99.2%, about 99.3%, about 99.4%, about 99.5%, about 99.6%, about 99.7%, about 99.8%, about 99.9%, about 99.92%, about99.94%, about 99.96%, about 99.98%, or about 100%, including all values and sub ranges in between. In some embodiments, a purity of the produced lithium metal electrode is at least 90%, at least 91%, at least 92%, at least 93%, at least 94%, at least 95%, at least 96%, at least 97%, at least 97.5%, at least 98%, at least 98.2%, at least 98.4%, at least 98.6%, at least 98.8%, at least 99%, at least 99.1%, at least 99.2%, at least 99.3%, at least 99.4%, at least 99.5%, at least 99.6%, at least 99.7%, at least 99.8%, at least 99.9%, at least 99.92%, at least 99.94%, at least 99.96%, at least 99.98%, or at least 100%. In some embodiments, a purity of the produced lithium metal electrode is at most 90%, at most 91%, at most 92%, at most 93%, at most 94%, at most 95%, at most 96%, at most 97%, at most 97.5%, at most 98%, at most 98.2%, at most 98.4%, at most 98.6%, at most 98.8%, at most 99%, at most 99.1%, at most 99.2%, at most 99.3%, at most 99.4%, at most 99.5%, at most 99.6%, at most 99.7%, at most 99.8%, at most 99.9%, at most 99.92%, at most 99.94%, at most 99.96%, at most 99.98%, or at most 100%.

[0288] In some embodiments, the lithium-rich intermediate electrode can be delithiated at the second widget and returned to the first widget as many times as possible.

[0289] In some embodiments, the produced lithium metal electrode can be treated by refining or post processes. In some embodiments, the refining or post processes comprise cleaning, heating, calendaring, or applying pressure on the electrode. In some embodiments, the produced lithium metal electrode can be heated at a temperature below about 150°C. In some embodiments, the produced lithium metal electrode can be heated at a temperature of 100°C, 110°C, 120°C, 130°C, 140°C, 150°C, 160°C, 170°C, or 180°C. In some embodiments, the produced lithium metal electrode can be heated at a temperature of about 100°C, about 110°C, about 120°C, about 130°C, about 140°C, about 150°C, about 160°C, about 170°C, or about 180°C. In some embodiments, the produced lithium metal electrode can be heated at a temperature of at least 100°C, at least 110°C, at least 120°C, at least 130°C, at least 140°C, at least 150°C, at least 160°C, at least 170°C, or at least 180°C. In some embodiments, the produced lithium metal electrode can be heated at a temperature of at most 100°C, at most 110°C, at most 120°C, at most 130°C, at most 140°C, at most 150°C, at most 160°C, at most 170°C, or at most 180°C.

[0290] In some embodiments, the produced lithium metal electrode can be treated by pressure at most 5 MPa. In some embodiments, the produced lithium metal electrode can be treated by pressure of 1 MPa, 2 MPa, 3 MPa, 4 MPa, 5 MPa, 6 MPa, 7 MPa, or 8 MPa. In some embodiments, the produced lithium metal electrode can be treated by pressure of about 1 MPa, about 2 MPa, about 3 MPa, about 4 MPa, about 5 MPa, about 6 MPa, about 7 MPa, or about 8 MPa. In some embodiments, the produced lithium metal electrode can be treated by pressure ofat least 1 MPa, at least 2 MPa, at least 3 MPa, at least 4 MPa, at least 5 MPa, at least 6 MPa, at least 7 MPa, or at least 8 MPa. In some embodiments, the produced lithium metal electrode can be treated by pressure of at most 1 MPa, at most 2 MPa, at most 3 MPa, at most 4 MPa, at most 5 MPa, at most 6 MPa, at most 7 MPa, or at most 8 MPa.

[0291] In some embodiments, the counter electrode, the intermediate electrode, and / or the current collector substrate can be in a roll form. In some embodiments, the counter electrode can be in a roll form. In some embodiments, the intermediate electrode can be in a roll form. In some embodiments, the current collector substrate can be in a roll form.

[0292] In some embodiments, the second widget further comprises a roll-to-roll production part.

[0293] In some embodiments, the system can be used for a scale-up production.

[0294] In some embodiments, the system can be configured to repeatedly produce a lithium metal electrode from one lithium rich intermediate electrode.

[0295] FIG. 13 illustrates a flow chart of the process. Initially, a lithium feedstock (14A) and an FP electrode (14B) can be prepared. The feedstock and the FP electrode can be subjected to an electro-absorption step (14C) under a buffer solution (14D) and an applied electric field (14E), which can result in the production of an LFP electrode (14F). This newly formed LFP electrode can then be rinsed and dried (14G) in preparation for the subsequent electro-deposition step (14H). Concurrently, the electrolyte (141) used in the electro-deposition phase can be recycled through an electrolyte recovery process ( 14 J). The electro-deposition step can be carried out under an inert atmosphere, using electricity(14L), a separator (14K), and a copper current collector (14M). Following the generation of the lithium electrode, a post-treatment phase can ensue via a calendaring process (14N). Once the post-treatment phase is completed, the electrode can be prepared for packaging (140). The pH of the buffer solution (14D) can play a role in preserving the structural integrity of the intermediate electrode material. As an illustration, in the case of Lithium Iron Phosphate (LFP), the pH can be consistently sustained between a range of about 7 to about 10 to uphold its efficacy. In some embodiments, the pH can be 6, 7, 8, 9, 10, or 11. In some embodiments, the pH can be at least 6, at least 7, at least 8, at least 9, at least 10, or at least 11. In some embodiments, the pH can be at most 6, at most 7, at most 8, at most 9, at most 10, or at most 11. In some embodiments, the pH can be about 6, about 7, about 8, about 9, about 10, or about 11. This pH balance can be achieved through several methods. One method can involve the use of a buffer such as potassium hydroxide (KOH), known for its alkaline nature and stability. An alternative approach can be the utilization of lithium hydroxide (Li OH) as the source of lithium, which not only furnishes the required lithium for the process but alsoassists in maintaining the desired pH range. Furthermore, segregating the anode chamber from the brine using an anion exchange membrane can present another viable solution. This process can control pH levels, ensuring the successful operation of the intermediate electrode material. The generation of an electric field, denoted by reference number 14E, is facilitated through the employment of a potentiostat. The device functions to maintain a steady current or voltage in order to prevent the occurrence of hydrogen evolution at the intermediate electrode (~0V vs. NHE). To prevent the oxidative decay of the lithium iron phosphate (LFP), the electric potential, denoted by reference number 14L, is meticulously regulated to remain under the threshold of 4V. The electrolyte recovery, referenced as 14 J, can be performed using solvent recovery techniques, which include but not limited to procedures such as rinsing, distillation, or the application of mechanical pressure.

[0296] The electrolyte recovery process (14J) can be carried out through several methods. In some embodiments, it includes the use of solvent extraction processes. The solvent extraction process involves the use of an organic solvent to extract the electrolyte from the electrodeposition process (14H), where the electrolyte dissolves into the solvent. In some embodiments, an organic solvent, such as ethylene carbonate, can be introduced, which aids in dissolving the electrolyte components. Following extraction, the solvent can be separated from the residual solid waste using filtration or centrifugation methods. The solvent, now containing the dissolved electrolyte, can be then subjected to evaporation, in some cases, under reduced pressure or elevated temperatures, leading to the recovery of electrolyte components. As a last step, the recovered electrolyte can be subjected to purification processes, such as fractional distillation or crystallization, to ensure its quality for reuse (141).

[0297] In some embodiments, the recovery of electrolytes ( 14 J) involves the use of supercritical carbon dioxide extraction. It employs carbon dioxide (CO2) at a state where it exhibits properties of both liquid and gas, known as the supercritical state. After the extraction process, the reduction of temperature and pressure transforms the supercritical CO2 back into its gaseous state, leaving behind the extracted electrolyte (141).

[0298] In some embodiments, the recovery of electrolytes ( 14J) can be performed by distillation or crystallization. It involves heating the used electrolyte to evaporate the electrolyte. This evaporated electrolyte can be then channeled into a condensing system, where it is cooled down. Upon cooling, the electrolyte components condense back into their liquid state and can be collected. In some embodiments, crystallization techniques can be employed. The cooledelectrolyte solution can be further cooled to below its solubility limit, causing the electrolyte components to form crystals that can be easily collected (141).

[0299] The systems and methods described in the present disclosure can be efficiently implemented within a manufacturing facility. One major advantage can be that the lithium metal electrodes produced can be seamlessly integrated into an existing battery manufacturing process. This could potentially streamline the production process, reducing operational complexity and enhancing the speed of production.

[0300] In certain embodiments, all steps of the method are conducted within a single manufacturing facility. This could facilitate easy coordination between different stages of the process, eliminate the need for transportation between facilities, and potentially reduce manufacturing costs. Moreover, this facility can be compact, contained within an area of no more than 10 km2, or even less than about 1 km2. In some embodiments, an area of the facility can be no more than 10 km2. In some embodiments, an area of the facility can be less than about 1 km2.

[0301] In certain embodiments, the manufacturing facility can be operatively connected to a battery facility dedicated to the construction of lithium metal batteries. This combination allows for a streamlined transition from the production of lithium metal electrodes to their incorporation into batteries. With the integration of the battery facility, the total area required for both facilities can remain compact, occupying no more than 10 km2, and in some instances, less than 1 km2. In some embodiments, the total area required for both facilities can be no more than 10 km2. In some embodiments, the total area required for both facilities can be less than about 1 km2.COMPUTING SYSTEM

[0302] In some aspects, the present disclosure describes a computer-implemented system comprising: a digital processing device comprising: at least one processor, an operating system configured to perform executable instructions, a memory, and a computer program including instructions executable by the digital processing device to operate a system for extracting lithium from brine. In some aspects, the present disclosure describes a computer-implemented method, implementing any one of the methods disclosed herein in a computer system. Referring to FIG. 6, a block diagram is shown depicting an exemplary machine that includes a computer system 1000 (e.g., a processing or computing system) within which a set of instructions can execute for causing a device to perform or execute any one or more of the aspects and / or methodologies for operating a system for extracting lithium from brine. The components in FIG. 6 are examples only and do not limit the scope of use or functionality of any hardware, software, embeddedlogic component, or a combination of two or more such components implementing particular embodiments.

[0303] Computer system 1000 can include one or more processors 1001, a memory 1003, and a storage 1008 that communicate with each other, and with other components, via a bus 1040. The bus 1040 may also link a display 1032, one or more input devices 1033 (which may, for example, include a keypad, a keyboard, a mouse, a stylus, etc.), one or more output devices 1034, one or more storage devices 1035, and various tangible storage media 1036. All of these elements may interface directly or via one or more interfaces or adaptors to the bus 1040. For instance, the various tangible storage media 1036 can interface with the bus 1040 via storage medium interface 1026. Computer system 1000 may have any suitable physical form, including but not limited to one or more integrated circuits (ICs), printed circuit boards (PCBs), mobile handheld devices (such as mobile telephones or PDAs), laptop or notebook computers, distributed computer systems, computing grids, or servers.

[0304] Computer system 1000 includes one or more processor(s) 1001 (e.g., central processing units (CPUs), general purpose graphics processing units (GPGPUs), or quantum processing units (QPUs)) that carry out functions. Computer system 1000 may be one of various high performance computing platforms. For instance, the one or more processor(s) 1001 may form a high performance computing cluster. In some embodiments, the one or more processors 1001 may form a distributed computing system connected by wired and / or wireless networks. In some embodiments, arrays of CPUs, GPUs, QPUs, or any combination thereof may be operably linked to implement any one of the methods disclosed herein. Processor(s) 1001 optionally contains a cache memory unit 1002 for temporary local storage of instructions, data, or computer addresses. Processor(s) 1001 are configured to assist in execution of computer readable instructions. Computer system 1000 may provide functionality for the components depicted in FIG. 6 as a result of the processor(s) 1001 executing non-transitory, processor-executable instructions embodied in one or more tangible computer-readable storage media, such as memory 1003, storage 1008, storage devices 1035, and / or storage medium 1036. The computer-readable media may store software that implements particular embodiments, and processor(s) 1001 may execute the software. Memory 1003 may read the software from one or more other computer-readable media (such as mass storage device(s) 1035, 1036) or from one or more other sources through a suitable interface, such as network interface 1020. The software may cause processor(s) 1001 to carry out one or more processes or one or more steps of one or more processes described orillustrated herein. Carrying out such processes or steps may include defining data structures stored in memory 1003 and modifying the data structures as directed by the software.

[0305] The memory 1003 may include various components (e.g., machine readable media) including, but not limited to, a random access memory component (e.g., RAM 1004) (e.g., static RAM (SRAM), dynamic RAM (DRAM), ferroelectric random access memory (FRAM), phasechange random access memory (PRAM), etc.), a read-only memory component (e.g., ROM 1005), and any combinations thereof. ROM 1005 may act to communicate data and instructions unidirectionally to processor(s) 1001, and RAM 1004 may act to communicate data and instructions bidirectionally with processor(s) 1001. ROM 1005 and RAM 1004 may include any suitable tangible computer-readable media described below. In one example, a basic input / output system 1006 (BIOS), including basic routines that help to transfer information between elements within computer system 1000, such as during start-up, may be stored in the memory 1003.

[0306] Fixed storage 1008 is connected bidirectionally to processor(s) 1001, optionally through storage control unit 1007. Fixed storage 1008 provides additional data storage capacity and may also include any suitable tangible computer-readable media described herein. Storage 1008 may be used to store operating system 1009, executable(s) 1010, data 1011, applications 1012 (application programs), and the like. Storage 1008 can also include an optical disk drive, a solid- state memory device (e.g., flash-based systems), or a combination of any of the above. Information in storage 1008 may, in appropriate cases, be incorporated as virtual memory in memory 1003.

[0307] In one example, storage device(s) 1035 may be removably interfaced with computer system 1000 (e.g., via an external port connector (not shown)) via a storage device interface 1025. Particularly, storage device(s) 1035 and an associated machine-readable medium may provide non-volatile and / or volatile storage of machine-readable instructions, data structures, program modules, and / or other data for the computer system 1000. In one example, software may reside, completely or partially, within a machine-readable medium on storage device(s) 1035. In another example, software may reside, completely or partially, within processor(s) 1001.

[0308] Bus 1040 connects a wide variety of subsystems. Herein, reference to a bus may encompass one or more digital signal lines serving a common function, where appropriate. Bus 1040 may be any of several types of bus structures including, but not limited to, a memory bus, a memory controller, a peripheral bus, a local bus, and any combinations thereof, using any of a variety of bus architectures. As an example, and not by way of limitation, such architecturesinclude an Industry Standard Architecture (ISA) bus, an Enhanced ISA (EISA) bus, a Micro Channel Architecture (MCA) bus, a Video Electronics Standards Association local bus (VLB), a Peripheral Component Interconnect (PCI) bus, a PCI-Express (PCI-X) bus, an Accelerated Graphics Port (AGP) bus, HyperTransport (HTX) bus, serial advanced technology attachment (SATA) bus, and any combinations thereof.

[0309] Computer system 1000 may also include an input device 1033. In one example, a user of computer system 1000 may enter commands and / or other information into computer system 1000 via input device(s) 1033. Examples of an input device(s) 1033 include, but are not limited to, an alpha-numeric input device (e.g., a keyboard), a pointing device (e.g., a mouse or touchpad), a touchpad, a touch screen, a multi-touch screen, a joystick, a stylus, a gamepad, an audio input device (e.g., a microphone, a voice response system, etc.), an optical scanner, a video or still image capture device (e.g., a camera), and any combinations thereof. In some embodiments, the input device is a Kinect, Leap Motion, or the like. Input device(s) 1033 may be interfaced to bus 1040 via any of a variety of input interfaces 1023 (e.g., input interface 1023) including, but not limited to, serial, parallel, game port, USB, FIREWIRE, THUNDERBOLT, or any combination of the above. In some embodiments, an input device 1033 may be used to operate a system for extracting lithium from brine. In some embodiments, a computer- implemented method comprises using human inputs through an input device 1033.

[0310] In particular embodiments, when computer system 1000 is connected to network 1030, computer system 1000 may communicate with other devices, specifically mobile devices and enterprise systems, distributed computing systems, cloud storage systems, cloud computing systems, and the like, connected to network 1030. Communications to and from computer system 1000 may be sent through network interface 1020. For example, network interface 1020 may receive incoming communications (such as requests or responses from other devices) in the form of one or more packets (such as Internet Protocol (IP) packets) from network 1030, and computer system 1000 may store the incoming communications in memory 1003 for processing. Computer system 1000 may similarly store outgoing communications (such as requests or responses to other devices) in the form of one or more packets in memory 1003 and communicated to network 1030 from network interface 1020. Processor(s) 1001 may access these communication packets stored in memory 1003 for processing.

[0311] Examples of the network interface 1020 include, but are not limited to, a network interface card, a modem, and any combination thereof. Examples of a network 1030 or network segment 1030 include, but are not limited to, a distributed computing system, a cloud computingsystem, a wide area network (WAN) (e.g., the Internet, an enterprise network), a local area network (LAN) (e.g., a network associated with an office, a building, a campus or other relatively small geographic space), a telephone network, a direct connection between two computing devices, a peer-to-peer network, and any combinations thereof. A network, such as network 1030, may employ a wired and / or a wireless mode of communication. In general, any network topology may be used.

[0312] Information and data can be displayed through a display 1032. Examples of a display 1032 include, but are not limited to, a cathode ray tube (CRT), a liquid crystal display (LCD), a thin film transistor liquid crystal display (TFT-LCD), an organic liquid crystal display (OLED) such as a passive-matrix OLED (PMOLED) or active-matrix OLED (AMOLED) display, a plasma display, and any combinations thereof. The display 1032 can interface to the processor(s) 1001, memory 1003, and fixed storage 1008, as well as other devices, such as input device(s) 1033, via the bus 1040. The display 1032 is linked to the bus 1040 via a video interface 1022, and transport of data between the display 1032 and the bus 1040 can be controlled via the graphics control 1021. In some embodiments, the display is a video projector. In some embodiments, the display is a head-mounted display (HMD) such as a VR headset. In further embodiments, suitable VR headsets include, by way of non-limiting examples, HTC Vive, Oculus Rift, Samsung Gear VR, Microsoft HoloLens, Razer OSVR, FOVE VR, Zeiss VR One, Avegant Glyph, Freefly VR headset, and the like. In still further embodiments, the display is a combination of devices such as those disclosed herein.

[0313] In addition to a display 1032, computer system 1000 may include one or more other peripheral output devices 1034 including, but not limited to, an audio speaker, a printer, a storage device, and any combinations thereof. Such peripheral output devices may be connected to the bus 1040 via an output interface 1024. Examples of an output interface 1024 include, but are not limited to, a serial port, a parallel connection, a USB port, a FIREWIRE port, a THUNDERBOLT port, and any combinations thereof.

[0314] In addition, or as an alternative, computer system 1000 may provide functionality as a result of logic hardwired or otherwise embodied in a circuit, which may operate in place of or together with software to execute one or more processes or one or more steps of one or more processes described or illustrated herein. Reference to software in this disclosure may encompass logic, and reference to logic may encompass software. Moreover, reference to a computer- readable medium may encompass a circuit (such as an IC) storing software for execution, acircuit embodying logic for execution, or both, where appropriate. The present disclosure encompasses any suitable combination of hardware, software, or both.

[0315] Those of skill in the art will appreciate that the various illustrative logical blocks, modules, circuits, and algorithm steps described in connection with the embodiments disclosed herein may be implemented as electronic hardware, computer software, or combinations of both. To clearly illustrate this interchangeability of hardware and software, various illustrative components, blocks, modules, circuits, and steps have been described above generally in terms of their functionality.

[0316] The various illustrative logical blocks, modules, and circuits described in connection with the embodiments disclosed herein may be implemented or performed with a general purpose processor, a digital signal processor (DSP), an application specific integrated circuit (ASIC), a field programmable gate array (FPGA) or other programmable logic device, discrete gate or transistor logic, discrete hardware components, or any combination thereof designed to perform the functions described herein. A general purpose processor may be a microprocessor, but in the alternative, the processor may be any conventional processor, controller, microcontroller, or state machine. A processor may also be implemented as a combination of computing devices, e.g., a combination of a DSP and a microprocessor, a plurality of microprocessors, one or more microprocessors in conjunction with a DSP core, or any other such configuration.

[0317] The steps of a method or algorithm described in connection with the embodiments disclosed herein may be embodied directly in hardware, in a software module executed by one or more processor(s), or in a combination of the two. A software module may reside in RAM memory, flash memory, ROM memory, EPROM memory, EEPROM memory, registers, hard disk, a removable disk, a CD-ROM, or any other form of storage medium known in the art. An exemplary storage medium is coupled to the processor such the processor can read information from, and write information to, the storage medium. In the alternative, the storage medium may be integral to the processor. The processor and the storage medium may reside in an ASIC. The ASIC may reside in a user terminal. In the alternative, the processor and the storage medium may reside as discrete components in a user terminal.

[0318] In accordance with the description herein, suitable computing devices include, by way of non-limiting examples, server computers, desktop computers, laptop computers, notebook computers, sub-notebook computers, netbook computers, netpad computers, set-top computers, media streaming devices, handheld computers, Internet appliances, mobile smartphones, and tablet computers.

[0319] In some embodiments, the computing device includes an operating system configured to perform executable instructions. The operating system is, for example, software, including programs and data, which manages the device’s hardware and provides services for execution of applications. Those of skill in the art will recognize that suitable server operating systems include, by way of non -limiting examples, FreeBSD, OpenBSD, NetBSD®, Linux, Apple® Mac OS X Server®, Oracle® Solaris®, Windows Server®, and Novell® NetWare®. Those of skill in the art will recognize that suitable personal computer operating systems include, by way of nonlimiting examples, Microsoft® Windows®, Apple® Mac OS X®, UNIX®, and UNIX-like operating systems such as GNU / Linux®. In some embodiments, the operating system is provided by cloud computing. Those of skill in the art will also recognize that suitable mobile smartphone operating systems include, by way of non-limiting examples, Nokia® Symbian® OS, Apple® los®, Research In Motion® BlackBerry OS®, Google® Android®, Microsoft® Windows Phone® OS, Microsoft® Windows Mobile® OS, Linux®, and Palm® WebOS®.

[0320] In some embodiments, a computer system 1000 may be accessible through a user terminal to receive user commands. The user commands may include line commands, scripts, programs, etc., and various instructions executable by the computer system 1000. A computer system 1000 may receive instructions to operate a system for extracting lithium from brine, or to schedule a computing job for the computer system 1000 to carry out any instructions.NON-TRANSITORY COMPUTER READABLE STORAGE MEDIUM

[0321] In some aspects, the present disclosure describes a non-transitory computer-readable storage media encoded with a computer program including instructions executable by one or more processors to operate a system for extracting lithium from brine using any one of the methods disclosed herein. In some embodiments, a non-transitory computer-readable storage media may comprise instructions for operating a system for extracting lithium from brine. In some embodiments, the platforms, systems, media, and methods disclosed herein include one or more non-transitory computer readable storage media encoded with a program including instructions executable by the operating system of an optionally networked computing device.

[0322] In further embodiments, a computer readable storage medium is a tangible component of a computing device. In still further embodiments, a computer readable storage medium is optionally removable from a computing device. In some embodiments, a computer readable storage medium includes, by way of non-limiting examples, flash memory devices, solid state memory, magnetic disk drives, magnetic tape drives, optical disk drives, distributed computing systems including cloud computing systems and services, and the like. In some embodiments,the program and instructions are permanently, substantially permanently, semi-permanently, or non-transitorily encoded on the media.COMPUTER PROGRAM

[0323] In some aspects, the present disclosure describes a computer program product comprising a computer-readable medium having computer-executable code encoded therein, the computerexecutable code adapted to be executed to implement any one of the methods disclosed herein. In some embodiments, the platforms, systems, media, and methods disclosed herein include at least one computer program, or use of the same.

[0324] A computer program includes a sequence of instructions, executable by one or more processor(s) of the computing device’s CPU, written to perform a specified task. Computer readable instructions may be implemented as program modules, such as functions, objects, Application Programming Interfaces (APIs), computing data structures, and the like, that perform particular tasks or implement particular abstract data types. In light of the disclosure provided herein, those of skill in the art will recognize that a computer program may be written in various versions of various languages. In some embodiments, APIs may comprise various languages, for example, languages in various releases of TensorFlow, Theano, Keras, PyTorch, or any combination thereof which may be implemented in various releases of Python, Python3, C, C#, C++, MatLab, R, Java, or any combination thereof.

[0325] The functionality of the computer readable instructions may be combined or distributed as desired in various environments. In some embodiments, a computer program comprises one sequence of instructions. In some embodiments, a computer program comprises a plurality of sequences of instructions. In some embodiments, a computer program is provided from one location. In other embodiments, a computer program is provided from a plurality of locations. In various embodiments, a computer program includes one or more software modules. In various embodiments, a computer program includes, in part or in whole, one or more web applications, one or more standalone applications, one or more web browser plug-ins, extensions, add-ins, or add-ons, or combinations thereof.WEB APPLICATION

[0326] In some embodiments, a computer program includes a web application. In some embodiments, a user may enter a query for operating a system for extracting lithium from brine through a web application. In light of the disclosure provided herein, those of skill in the art will recognize that a web application, in various embodiments, utilizes one or more softwareframeworks and one or more database systems. In some embodiments, a web application is created upon a software framework such as Microsoft® .NET or Ruby on Rails (RoR). In some embodiments, a web application utilizes one or more database systems including, by way of nonlimiting examples, relational, non-relational, object oriented, associative, XML, and document oriented database systems. In further embodiments, suitable relational database systems include, by way of non-limiting examples, Microsoft® SQL Server, mySQL™, and Oracle®. Those of skill in the art will also recognize that a web application, in various embodiments, is written in one or more versions of one or more languages. A web application may be written in one or more markup languages, presentation definition languages, client-side scripting languages, server-side coding languages, database query languages, or combinations thereof. In some embodiments, a web application is written to some extent in a markup language such as Hypertext Markup Language (HTML), Extensible Hypertext Markup Language (XHTML), or extensible Markup Language (XML). In some embodiments, a web application is written to some extent in a presentation definition language such as Cascading Style Sheets (CSS). In some embodiments, a web application is written to some extent in a client-side scripting language such as Asynchronous JavaScript and XML (AJAX), Flash® ActionScript, JavaScript, or Silverlight®. In some embodiments, a web application is written to some extent in a server-side coding language such as Active Server Pages (ASP), ColdFusion®, Perl, Java™, JavaServer Pages (JSP), Hypertext Preprocessor (PHP), Python™, Ruby, Tel, Smalltalk, WebDNA®, or Groovy. In some embodiments, a web application is written to some extent in a database query language such as Structured Query Language (SQL). In some embodiments, a web application integrates enterprise server products such as IBM® Lotus Domino®.Mobile application

[0327] In some embodiments, a computer program includes a mobile application provided to a mobile computing device. In some embodiments, the mobile application is provided to a mobile computing device at the time it is manufactured. In other embodiments, the mobile application is provided to a mobile computing device via the computer network described herein.

[0328] In view of the disclosure provided herein, a mobile application is created by techniques known to those of skill in the art using hardware, languages, and development environments known to the art. Those of skill in the art will recognize that mobile applications are written in several languages. Suitable programming languages include, by way of non-limiting examples,C, C++, C#, Objective-C, Java™, JavaScript, Pascal, Object Pascal, Python™, Ruby, VB.NET, WML, and XHTML / HTML with or without CSS, or combinations thereof.

[0329] Suitable mobile application development environments are available from several sources. Commercially available development environments include, by way of non-limiting examples, AirplaySDK, alcheMo, Appcelerator®, Celsius, Bedrock, Flash Lite, .NET Compact Framework, Rhomobile, and WorkLight Mobile Platform. Other development environments are available without cost including, by way of non-limiting examples, Lazarus, MobiFlex, MoSync, and Phonegap. Also, mobile device manufacturers distribute software developer kits including, by way of non-limiting examples, iPhone and iPad (los) SDK, Android™ SDK, BlackBerry® SDK, BREW SDK, Palm® OS SDK, Symbian SDK, webOS SDK, and Windows® Mobile SDK.STANDALONE APPLICATION

[0330] In some embodiments, a computer program includes a standalone application, which is a program that is run as an independent computer process, not an add-on to an existing process, e.g., not a plug-in. Those of skill in the art will recognize that standalone applications are often compiled. A compiler is a computer program(s) that transforms source code written in a programming language into binary object code such as assembly language or machine code. Suitable compiled programming languages include, by way of non-limiting examples, C, C++, Objective-C, COBOL, Delphi, Eiffel, Java™, Lisp, Python™, Visual Basic, and VB .NET, or combinations thereof. Compilation is often performed, at least in part, to create an executable program. In some embodiments, a computer program includes one or more executable complied applications.SOFTWARE MODULES

[0331] In some embodiments, the platforms, systems, media, and methods disclosed herein include software, server, and / or database modules, or use of the same. In view of the disclosure provided herein, software modules are created by techniques known to those of skill in the art using machines, software, and languages known to the art. The software modules disclosed herein are implemented in a multitude of ways. In various embodiments, a software module comprises a file, a section of code, a programming object, a programming structure, a distributed computing resource, a cloud computing resource, or combinations thereof. In further various embodiments, a software module comprises a plurality of files, a plurality of sections of code, a plurality of programming objects, a plurality of programming structures, a plurality of distributed computing resources, a plurality of cloud computing resources, or combinations thereof. Invarious embodiments, the one or more software modules comprise, by way of non-limiting examples, a web application, a mobile application, a standalone application, and a distributed or cloud computing application. In some embodiments, software modules are in one computer program or application. In other embodiments, software modules are in more than one computer program or application. In some embodiments, software modules are hosted on one machine. In other embodiments, software modules are hosted on more than one machine. In further embodiments, software modules are hosted on a distributed computing platform such as a cloud computing platform. In some embodiments, software modules are hosted on one or more machines in one location. In other embodiments, software modules are hosted on one or more machines in more than one location.TERMINOLOGY

[0332] Unless defined otherwise, all terms of art, notations, and other technical and scientific terms or terminology used herein are intended to have the same meaning as is commonly understood by one of ordinary skill in the art to which the claimed subject matter pertains. In some cases, terms with commonly understood meanings are defined herein for clarity and / or for ready reference, and the inclusion of such definitions herein should not necessarily be construed to represent a substantial difference over what is generally understood in the art.

[0333] Throughout this application, various embodiments may be presented in a range of formats. It should be understood that the description in range format is merely for convenience and brevity and should not be construed as an inflexible limitation on the scope of the disclosure. Accordingly, the description of a range should be considered to have specifically disclosed all the possible subranges as well as individual numerical values within that range. For example, description of a range such as from 1 to 6 should be considered to have specifically disclosed subranges such as from 1 to 3, from 1 to 4, from 1 to 5, from 2 to 4, from 2 to 6, from 3 to 6 etc., as well as individual numbers within that range, for example, 1, 2, 3, 4, 5, and 6. This applies regardless of the breadth of the range.

[0334] As used in the specification and claims, the singular forms “a”, “an” and “the” include plural references unless the context clearly dictates otherwise. For example, the term “a sample” includes a plurality of samples, including mixtures thereof.

[0335] Whenever the term “at least,” “greater than,” or “greater than or equal to” precedes the first numerical value in a series of two or more numerical values, the term “at least,” “greater than” or “greater than or equal to” applies to each of the numerical values in that series ofnumerical values. For example, greater than or equal to 1, 2, or 3 is equivalent to greater than or equal to 1, greater than or equal to 2, or greater than or equal to 3.

[0336] Whenever the term “no more than,” “less than,” or “less than or equal to” precedes the first numerical value in a series of two or more numerical values, the term “no more than,” “less than,” or “less than or equal to” applies to each of the numerical values in that series of numerical values. For example, less than or equal to 3, 2, or 1 is equivalent to less than or equal to 3, less than or equal to 2, or less than or equal to 1.

[0337] The expression “about A to B and C to D” may be construed to mean between about A and about B and between about C and about D. The expression “about A to B or C to D” may be construed to mean between about A and about B or between about C and about D.

[0338] The term “exemplary” as used herein means “serving as an example, instance, or illustration.” Any embodiment described herein as “exemplary” is not to be construed as preferred or advantageous over other embodiments.

[0339] As used herein, the term “about” a number refers to that number plus or minus 10% of that number. The term “about” a range refers to that range minus 10% of its lowest value and plus 10% of its greatest value.

[0340] As used herein, the term “conductive substrate” can refer to an electrically conductive material that can function as a cathode in an electrolytic cell.

[0341] As used herein, the term “brine” can refer to an aqueous salt solution. The terms “brine” and “aqueous phase” can be used interchangeably.

[0342] As used herein, the term “carbon cloth” can refer to a textile material composed predominantly of carbon atoms. The carbon cloth is derived through the carbonization of a polymeric precursor, often polyacrylonitrile (PAN) or rayon, which is heated in a controlled environment to drive off non-carbon atoms and leave behind a network of pure carbon fibers.

[0343] The section headings used herein are for organizational purposes only and are not to be construed as limiting the subject matter described.

[0344] Various embodiments are described in more detail with reference to the accompanying drawings. The detailed descriptions are provided to assist the reader in gaining a comprehensive understanding of the methods, apparatuses, and / or systems described herein as well as modifications thereof. Accordingly, various modifications and equivalents of the methods, apparatuses, and / or systems described herein are apparent to those of ordinary skill in the art. Descriptions of well-known functions and constructions may be omitted for increased clarity and conciseness.EXAMPLEExample 1: Lithium Metal Battery (I)

[0345] The performance of refined lithium metal, which was disclosed herein, was evaluated by comparing with a commercial lithium when subjected to identical cycling conditions. These conditions involved a 1C: 1C charge to discharge ratio, an LFP of 1.25mAh / cm2, and a lithium anode of 20 pm. Additionally, the conditions included 300 pL of IM LiTFSI DOL DME with l%wt LiNO3.

[0346] Regarding specific discharge capacity, commercial lithium exhibited a decrease after around 300 cycles. In contrast, the specific discharge capacity of the lithium metal electrode disclosed herein exhibited a decrease after around 400 cycles. The experimental data is shown in FIG. 12Example : Lithium metal battery (II)

[0347] The lithium metal electrode, prepared through the method disclosed herein, was employed as an anode in the designed lithium battery configuration. Employing a lithium iron phosphate (LFP) cathode in conjunction with this anode, the configuration enhanced the energy density, reaching to 220 Wh / kg. Furthermore, it exhibited a cycle life extending over 1000 cycles.

[0348] As an additional embodiment, the lithium battery employed a cathode derived from vanadium oxide (VxOy) coupled with the lithium metal electrode, as prepared by the disclosed method, as an anode. The resulting battery configuration delivered an energy density of 400 Wh / kg, while maintaining a cycle life exceeding 1000 cycles.

[0349] Traditional batteries utilizing a LFP cathode paired with a composite anode of graphite and silicon (2%) yielded an energy density of 180 Wh / kg. Similarly, existing battery configuration utilizing a cathode of NMC-811 (Lithium Nickel Manganese Cobalt Oxide (LiNio.8Mno.1Coo.1O2)) paired with an extruded lithium metal anode, were limited to a cycle life of just 600 cycles. Compared to a configuration involving a sulfur-graphene composite cathode and lithium metal / graphite anode combination, which provides an energy density of 248 Wh / kg but has a restricted cycle life of 230 cycles, the lithium battery configurations with lithium metal electrode prepared by the disclosed method established their superiority. This superiority is established in terms of both enhanced energy density and extended cycle life, outperforming existing technologies in these critical parameters.

[0350] While preferred embodiments of the present disclosure have been shown and described herein, it will be obvious to those skilled in the art that such embodiments are provided by way of example only. Numerous variations, changes, and substitutions will now occur to those skilled in the art without departing from the disclosure. It should be understood that various alternatives to the embodiments of the disclosure described herein may be employed in practicing the disclosure. It is intended that the following claims define the scope of the disclosure and that methods and structures within the scope of these claims and their equivalents be covered thereby.

Claims

CLAIMSWhat is claimed is:

1. A method comprising:(i) contacting an intermediate electrode with an aqueous source comprising lithium;(ii) extracting and transferring the lithium from the aqueous source to the intermediate electrode to form a lithium-rich intermediate electrode; and(iii) transferring the lithium from the lithium-rich intermediate electrode to a current collector substrate to form an electrode for a rechargeable energy device.

2. A method comprising:(i) contacting an intermediate electrode with an aqueous source comprising lithium;(ii) extracting and transferring the lithium from the aqueous source to the intermediate electrode to form a lithium-rich intermediate electrode; and(iii) transferring the lithium from the lithium-rich intermediate electrode to a current collector substrate to form an electrode for a rechargeable energy device, wherein the intermediate electrode is physically separated from the current collector substrate by a separator.

3. The method of claim 1 or 2, wherein the aqueous source comprising lithium is brine.

4. The method of any one of claims 1 to 3, wherein the aqueous source comprising lithium further comprises Na+, K+, Mg2+, Ca2+, B(0H)4 , Fe2+, Fe3+, Mn2+, MnCh2, MnO4, Cl’, SO42', NH3, NH4+, NH4OH, NO2, HNO2, NOs’, an alkali metal ion, an alkali earth metal ion, or any combination thereof.

5. The method of any one of claims 1 to 4, wherein the aqueous source comprising lithium comprises a geological resource.

6. The method of any one of claims 1 to 5, wherein the aqueous source comprising lithium is pretreated to remove Na+, K+, Mg2+, Ca2+, B(OH)4 , Fe2+, Fe3+, Mn2+, MnO42, MnO4", Cl’, SCU2’ , NH3, NH4+, NH4OH, NO2, HNO2, NO3’, an alkali metal ion, an alkali earth metal ion, or any combination thereof.

7. The method of any one of claims 1 to 6, wherein (ii) is performed by connecting a counter electrode to the intermediate electrode in a circuit, using the aqueous source comprising lithium as an electrolyte.

8. The method of any one of claims 1 to 7, wherein (iii) is performed by applying an electric potential across the lithium-rich intermediate electrode and the current collector substrate.

9. The method of any one of claims 1 to 8, wherein the intermediate electrode in (i) is substantially free of lithium or is in a de-lithiated state.

10. The method of claim 9, wherein the intermediate electrode comprises about 30 atomic % (at%) less than a maximum amount of lithium that can be present, before contacting with an aqueous source comprising lithium.

11. The method of any one of claims 1 to 10, wherein the intermediate electrode is obtained from recycled lithium-ion battery materials.

12. The method of claim 11, wherein the intermediate electrode is obtained from black mass produced from shredding lithium-ion battery materials.

13. The method of any one of claims 1 to 12, wherein the intermediate electrode comprises iron phosphate, manganese oxide, nickel manganese cobalt oxide, or any combination thereof.

14. The method of any one of claims 1 to 13, wherein the intermediate electrode comprises a metal current collector or a carbon current collector.

15. The method of claim 14, wherein the intermediate electrode comprises the metal current collector.

16. The method of claim 15, wherein the metal current collector comprises titanium (Ti), aluminum (Al), magnesium (Mg), copper (Cu), zinc (Zn), tin (Sn), vanadium oxide (V2O5), or any metal that is capable of forming an alloy with lithium.

17. The method of claim 15, wherein the metal current collector substrate comprises Cu-Ni, Cu- Ti, Cu-Zn, Cu-Al, Cu-Sn, Ni-CO, Al -Mg, Fe-Cr-Ni, or any combination thereof.

18. The method of claim 14, wherein the intermediate electrode comprises the carbon current collector.

19. The method of claim 18, wherein the carbon current collector comprises graphite or carbon cloth.

20. The method of any one of claims 1 to 19, wherein the intermediate electrode comprises an electrically conductive slurry comprising an electrically conductive additive.

21. The method of claim 20, wherein the electrically conductive additive comprises carbon.

22. The method of any one of claims 1 to 21, wherein the intermediate electrode is non-reactive with non-lithium components in the aqueous source.

23. The method of any one of claims 1 to 22, wherein the intermediate electrode is reactive with non-lithium components in the aqueous source.

24. The method of claim 23, wherein the intermediate electrode and a nonaqueous / polymer electrolyte are physically separated from a counter electrode and the aqueous source comprising lithium by the separator during extracting and transferring the lithium from the aqueous source to the intermediate electrode to form a lithium-rich intermediate electrode.

25. The method of claim 24, wherein the separator comprises a composite membrane comprising a lithium ion conductive polymer.

26. The method of claim 24, wherein the separator comprises a lithium ion-selective membrane.

27. The method of claim 24, wherein the lithium ion-selective membrane permits lithium ions to selectively flow through to the intermediate electrode.

28. The method of any one of claims 1 to 27, wherein the lithium-rich intermediate electrode comprises lithium iron phosphate (LiFePCU, LFP), lithium nickel manganese cobalt oxide (LiNiMnCoCh, NMC), lithium manganate (Li2MnO4, LMO), LiCe, LixMgy, LixAly, LixSiy, or a combination thereof.

29. The method of any one of claims 1 to 28, wherein transferring the lithium from the aqueous source to the intermediate electrode in (ii) comprises intercalating the lithium in the intermediate electrode to form the lithium-rich intermediate electrode.

30. The method of any one of claims 1 to 29, wherein the lithium-rich intermediate electrode comprises at least 30 at% more than a minimum amount of lithium that can be present.

31. The method of any one of claims 1 to 30, wherein transferring the lithium from the lithium- rich intermediate electrode to the current collector substrate in (iii) comprises delithiating the lithium-rich intermediate electrode.

32. The method of any one of claims 30 to 31, wherein the intercalating and the delithiating are reversible.

33. The method of any one of claims 1 to 32, wherein the current collector substrate comprises copper, copper alloy, aluminum, aluminum alloy, titanium, titanium alloy, nickel, nickel alloy, stainless steel, carbonaceous material, or any combination thereof.

34. The method of any one of claims 1 to 32, wherein the current collector substrate comprises Cu-Ni, Cu-Ti, Cu-Zn, Cu-Al, Cu-Sn, Ni-CO, Al -Mg, Fe-Cr-Ni, or any combination thereof.

35. The method of any one of claims 1 to 32, wherein the current collector substrate comprises carbon, carbon paper, carbon cloth or a metal or noble metal mesh or foil.

36. The method of any one of claims 1 to 35, wherein the current collector substrate comprises a foil, a mesh, a cloth, or a foam.

37. The method of any one of claims 1 to 36, wherein an electrical connection to the intermediate electrode is made via copper, copper alloy, aluminum, aluminum alloy, titanium, titanium alloy, nickel, nickel alloy, stainless steel, carbonaceous material, or any combination thereof.

38. The method of any one of claims 1 to 37, wherein the transferring of the lithium from the lithium-rich intermediate electrode to the current collector substrate comprises electrodeposition of the lithium as a layer of lithium metal on the current collector substrate.

39. The method of any one of claims 1 to 38, wherein the electrode is a battery-ready electrode.

40. The method of any one of claims 1 to 39, wherein (i) and (ii) are carried out in a first chamber and (iii) is carried out in a second chamber that is different from the first chamber.

41. The method of any one of claims 1 to 40, wherein the intermediate electrode is delithiated after (iii) and returned to the first chamber for repeating (i) and (ii).

42. The method of any one of claims 1 to 41, further comprising, after (ii) and before (iii), rinsing and / or drying the intermediate electrode.

43. The method of any one of claims 1 to 42, further comprising, after (iii), re-using the intermediate electrode in (i).

44. The method of any one of claims 1 to 43, further comprising, after (iii), treating the electrode by refining or post processes.

45. The method of claim 44, wherein the refining or post processes comprise cleaning, heating, or applying pressure on the electrode.

46. The method of claim 45, wherein the refining or post processes comprise applying heat to the electrode at a temperature below about 150°C.

47. The method of claim 45, wherein the refining or post processes comprise applying pressure on the electrode at most 5 MPa.

48. The method of any one of claims 1 to 47, wherein the counter electrode, the intermediate electrode, and / or the current collector substrate are in a roll form.

49. The method of any one of claims 1 to 48, wherein an electrode rolling press system is used.

50. The method of any one of claims 1 to 49 wherein the method is used for a scale-up production.

51. A system for producing an electrode comprising: a first chamber comprising: an aqueous source comprising lithium and an intermediate electrode, wherein the intermediate electrode is configured to extract and receive the lithium from the aqueous source to form a lithium-rich intermediate electrode; and a second chamber comprising a current collector substrate, wherein the lithium-rich intermediate electrode is configured to be transferred from the first chamber to the second chamber, and wherein the lithium from the lithium-rich intermediate electrode is transferred to the current collector substrate to form an electrode for a rechargeable energy device.

52. A system for producing an electrode comprising: a first chamber comprising: an aqueous source comprising lithium and an intermediate electrode, wherein the intermediate electrode is configured to extract and receive the lithium from the aqueous source to form a lithium-rich intermediate electrode; and a second chamber comprising a current collector substrate, wherein the lithium-rich intermediate electrode is configured to be transferred from the first chamber to the second chamber, wherein the lithium from the lithium-rich intermediate electrode is transferred to the current collector substrate to form an electrode for a rechargeable energy device, and wherein the intermediate electrode is physically separated from the current collector substrate by a separator.-HO-53. The system of claim 51 or 52, wherein the aqueous source comprising lithium is brine.

54. The system of any one of claims 51 to 53, wherein the aqueous source comprising lithium further comprises sodium, potassium, magnesium, calcium, boron, iron, manganese, chlorine, SO4, nitrogen, an alkali metal, an alkali earth metal, or any combination thereof.

55. The system of any one of claims 51 to 54, wherein the aqueous source comprising lithium comprises a geological resource.

56. The system of any one of claims 51 to 54, wherein the aqueous source comprising lithium is pretreated to remove magnesium, sodium, calcium, potassium, iron, boron, manganese, or any combination thereof.

57. The system of any one of claims 51 to 56, wherein the extracting and receiving the lithium from the aqueous source is performed by connecting a counter electrode to the intermediate electrode in a circuit, using the aqueous source comprising lithium as an electrolyte.

58. The system of any one of claims 51 to 57, wherein the lithium from the lithium-rich intermediate electrode is transferred to the current collector substrate by applying an electric potential across the lithium-rich intermediate electrode and the current collector substrate.

59. The system of any one of claims 51 to 58, wherein the intermediate electrode in (i) is substantially free of lithium or is in a de-lithiated state.

60. The system of claim 59, wherein the intermediate electrode comprises about 30 at% less than a maximum amount of lithium that can be present.

61. The system of any one of claims 51 to 60, wherein the intermediate electrode is obtained from recycled lithium-ion battery materials.

62. The system of claim 61, wherein the intermediate electrode is obtained from black mass produced from shredding of lithium-ion battery materials.

63. The system of any one of claims 51 to 62, wherein the intermediate electrode comprises iron phosphate, manganese oxide, or nickel manganese cobalt oxide.

64. The system of any one of claims 51 to 63, wherein the intermediate electrode comprises a metal current collector or a carbon current collector.

65. The system of claim 64, wherein the intermediate electrode comprises the metal current collector.

66. The system of claim 65, wherein the metal current collector comprises copper (Cu), titanium (Ti), aluminum (Al), magnesium (Mg), zinc (Zn), tin (Sn), vanadium oxide (V2O5), or any metal that is capable of forming an alloy with lithium.

67. The system of claim 65, wherein the metal current collector substrate comprises Cu-Ni, Cu- Ti, Cu-Zn, Cu-Al, Cu-Sn, Ni-CO, Al -Mg, Fe-Cr-Ni, or any combination thereof.

68. The system of claim 64, wherein the intermediate electrode comprises the carbon current collector.

69. The system of claim 68, wherein the carbon current collector comprises graphite or carbon cloth.

70. The system of any one of claims 51 to 69, wherein the intermediate electrode is non-reactive with non-lithium components in the aqueous source.

71. The system of any one of claims 51 to 70, wherein the intermediate electrode is reactive with non-lithium components in the aqueous source.

72. The system of claim 71, wherein the first chamber comprises the separator that physically separates the intermediate electrode and a nonaqueous / polymer electrolyte from a positive electrode and the aqueous source.

73. The system of claim 71, wherein the second chamber comprises the separator that physically separates the lithium-rich intermediate electrode and an electrolyte from a negative electrode and an aqueous source.

74. The system of claim 73, wherein the separator comprises a composite membrane comprising a lithium ion conductive polymer.

75. The system of any one of claims 51 to 74, wherein the separator comprises a lithium ion- selective membrane.

76. The system of claim 75, wherein the lithium ion-selective membrane permits lithium ions to selectively flow through.

77. The system of any one of claims 51 to 76, wherein the lithium-rich intermediate electrode comprises lithium iron phosphate (LiFePCU, LFP), lithium nickel manganese cobalt oxide (LiNiMnCoCh, NMC), lithium manganate (Li2MnO4, LMO), LiCe, LixMgy, LixAly, LixSiy, or a combination thereof.

78. The system of any one of claims 51 to 77, wherein the intermediate electrode is configured to receive the lithium from the aqueous source by intercalating the lithium in the intermediate electrode.

79. The system of any one of claims 51 to 78, wherein the lithium-rich intermediate electrode comprises at least 30 at% more than a minimum amount of lithium that can be present.

80. The system of any one of claims 51 to 79, wherein the lithium from the lithium-rich intermediate electrode is transferred to the current collector substrate by delithiating the lithium from the lithium-rich intermediate electrode.

81. The system of any one of claims 51 to 80, wherein the intercalating and the delithiating are reversible.

82. The system of any one of claims 51 to 81, wherein the current collector substrate comprises copper, copper alloy, aluminum, aluminum alloy, titanium, titanium alloy, nickel, nickel alloy, stainless steel, carbonaceous material, or any combination thereof.

83. The system of any one of claims 51 to 81, wherein the current collector substrate comprises Cu-Ni, Cu-Ti, Cu-Zn, Cu-Al, Cu-Sn, Ni-CO, Al -Mg, Fe-Cr-Ni, or any combination thereof.

84. The system of any one of claims 51 to 81, wherein the current collector substrate comprises carbon, carbon paper, carbon cloth or a metal or noble metal mesh or foil.

85. The system of any one of claims 51 to 84, wherein the current collector substrate comprises a foil, a mesh, a cloth, or a foam.

86. The system of any one of claims 51 to 85, wherein the lithium from the lithium-rich intermediate electrode is transferred to the current collector substrate by electrodeposition of the lithium as a layer of lithium metal on the current collector substrate.

87. The system of any one of claims 51 to 86, wherein the positive electrode, the intermediate electrode, and / or the current collector substrate are in a roll form.

88. A system for manufacturing a lithium metal electrode, comprising:(i) a first widget configured to contact an aqueous source comprising lithium with an intermediate electrode, thereby transferring the lithium to the intermediate electrode to form a lithium-rich intermediate electrode; and(ii) a second widget configured to transfer the lithium from the lithium-rich intermediate electrode to a current collector substrate to form the lithium metal electrode.

89. A system for manufacturing a lithium metal electrode, comprising:(i) a first widget configured to contact an aqueous source comprising lithium with an intermediate electrode, thereby transferring the lithium to the intermediate electrode to form a lithium-rich intermediate electrode; and(ii) a second widget configured to transfer the lithium from the lithium-rich intermediate electrode to a current collector substrate to form the lithium metal electrode, wherein the intermediate electrode is physically separated from the current collector substrate by a separator.

90. The system of claim 88 or 89, wherein the aqueous source comprising lithium is brine.

91. The system of any one of claims 88 to 90, wherein the aqueous source comprising Li+further comprisesNH3, NH4+, NH4OH, NO2, HNO2, NOs’, an alkali metal ions, an alkali earth metal ions, or any combination thereof.

92. The system of any one of claims 88 to 91, wherein the aqueous source comprising lithium comprises a geological resource.

93. The system of any one of claims 88 to 92, wherein the aqueous source comprising lithium is pretreated to remove, NH3, NH4+, NH4OH, NO2, HNO2, NO3’, an alkali metal ions, an alkali earth metal ions, or any combination thereof.

94. The system of any one of claims 88 to 93, wherein the first widget comprises a counter electrode.

95. The system of any one of claims 88 to 94, wherein in the first widget the intermediate electrode is connected with the counter electrode in a circuit, using the aqueous source comprising lithium as an electrolyte.

96. The system of any one of claims 88 to 95, wherein the second widget is configured to apply an electric potential across the lithium-rich intermediate electrode and the current collector substrate.

97. The system of any one of claims 88 to 96, wherein, before contacting the aqueous source comprising lithium, the intermediate electrode is substantially free of lithium or is in a de- lithiated state.

98. The system of any one of claims 88 to 97, wherein the intermediate electrode comprises about 30 atomic % (at%) less than a maximum amount of lithium that can be present.

99. The system of any one of claims 88 to 98, wherein the intermediate electrode is obtained from recycled lithium-ion battery materials.

100. The system of any one of claims 88 to 99, wherein the intermediate electrode is obtained from black mass produced from shredding lithium-ion battery materials.

101. The system of any one of claims 88 to 100, wherein the intermediate electrode comprises iron phosphate (FePCU), manganese oxide (MnCh), or nickel manganese cobalt oxide (NixMnyCoi-x-yCh).

102. The system of any one of claims 88 to 101, wherein the intermediate electrode comprises iron phosphate (FePO4).

103. The system of any one of claims 88 to 102, wherein the intermediate electrode comprises a metal current collector or a carbon current collector.

104. The system of any one of claims 88 to 103, wherein the intermediate electrode comprises the metal current collector.

105. The system of any one of claims 88 to 104, wherein the metal current collector comprises copper (Cu), titanium (Ti), aluminum (Al), magnesium (Mg), zinc (Zn), tin (Sn), vanadium oxide (V2O5), or any metal that is capable of forming an alloy with lithium.

106. The system of any one of claims 88 to 104, wherein the metal current collector substrate comprises Cu-Ni, Cu-Ti, Cu-Zn, Cu-Al, Cu-Sn, Ni-CO, Al-Mg, Fe-Cr-Ni, or any combination thereof.

107. The system of any one of claims 88 to 104, wherein the intermediate electrode comprises the carbon current collector.

108. The system of claim 107, wherein the carbon current collector comprises graphite or carbon cloth.

109. The system of any one of claims 88 to 108, wherein the first widget further comprises a roll- to-roll production part.

110. The system of any one of claims 88 to 109, wherein the first widget operates at temperatures up to about 95°C.11 l.The system of any one of claims 88 to 110, wherein the lithium-rich intermediate electrode comprises lithium iron phosphate (LiFePCU, LFP), lithium manganese oxide (LiMn2O4 spinel, or Li2MnO3-based lithium-rich layered materials, LMR-NMC), lithium nickel manganese cobalt oxide (LiNiMnCoCh or NMC), lithium manganate (Li2MnO4, LMO), LiCe, LixMgy, LixAly, LixSiy, or a combination thereof.

112. The system of any one of claims 88 to 111, wherein the lithium-rich intermediate electrode comprises lithium iron phosphate (LiFePCU, LFP).

113. The system of any one of claims 88 to 112, wherein the first widget is configured to transfer the lithium from the aqueous source to the intermediate electrode by intercalating the lithium in the intermediate electrode to form the lithium-rich intermediate electrode.

114. The system of any one of claims 88 to 113, wherein the lithium-rich intermediate electrode comprises at least 30 at% more than a minimum amount of lithium that can be present.

115. The system of any one of claims 88 to 114, wherein the lithium-rich intermediate electrode operates as a lithium ink.

116. The system of any one of claims 88 to 115, wherein the second widget is configured to transfer the lithium from the lithium-rich intermediate electrode to the current collector substrate by delithiating the lithium-rich intermediate electrode.

117. The system of any one of claims 88 to 116, wherein the intercalating and the delithiating are reversible.

118. The system of any one of claims 88 to 117, wherein the current collector substrate comprises copper, copper alloy, aluminum, aluminum alloy, titanium, titanium alloy, nickel, nickel alloy, stainless steel, carbonaceous material, or any combination thereof.

119. The system of any one of claims 88 to 118, wherein the current collector substrate comprises Cu.

120. The system of any one of claims 88 to 118, wherein the current collector substrate comprises Cu-Ni, Cu-Ti, Cu-Zn, Cu-Al, Cu-Sn, Ni-CO, Al -Mg, Fe-Cr-Ni, or any combination thereof.

121. The system of any one of claims 88 to 118, wherein the current collector substrate comprises carbon, carbon paper, carbon cloth or a metal or noble metal mesh or foil.

122. The system of any one of claims 88 to 118, wherein the current collector substrate comprises a foil, a mesh, a cloth, or a foam.

123. The system of any one of claims 88 to 122, wherein an electrical connection to the lithium- rich intermediate electrode is made via copper, copper alloy, aluminum, aluminum alloy, titanium, titanium alloy, nickel, nickel alloy, stainless steel, carbonaceous material, or any combination thereof.

124. The system of any one of claims 88 to 123, wherein the transferring of the lithium from the lithium-rich intermediate electrode to the current collector substrate comprises electrodeposition of the lithium as a layer of lithium metal on the current collector substrate.

125. The system of any one of claims 88 to 124, wherein the lithium is electrodeposited as a layer of lithium metal at least 1 micrometer (pm) thickness of a layer / min.

126. The system of any one of claims 88 to 125, wherein the electrodepositing comprises coating or printing the electrode ink on the current collector substrate.

127. The system of any one of claims 88 to 126, wherein the second widget operates at a temperature of about 10°C to about 150°C.

128. The system of any one of claims 88 to 127, wherein the second widget operates at a pressure of about 0.05 MPa to about 15 MPa.

129. The system of any one of claims 88 to 128, wherein the second widget operates at about 0.1 mA / cm2to about 50 mA / cm2.

130. The system of any one of claims 88 to 129, wherein the second widget comprises an electrolyte.

131. The system of any one of claims 88 to 130, wherein the electrolyte comprises (a) 1,3- di oxolane (DOL): 1, 2-dimeth oxy ethane (DME), 1 M lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), 1% LiNCh, (b) 2EC (ethylene carb onate): 3 EMC (ethyl methyl carbonate), 1 M LiTFSI, (c) tetraethylene glycol dimethyl ether (G4), 1 M LiNCE, or (d) diethylene glycol dimethyl ether (G2), 1 M LiNCE.

132. The system of any one of claims 88 to 131, wherein a boiling point of the electrolyte ranges from about 70°C to about 290°C.

133. The system of any one of claims 88 to 132, wherein the electrolyte is non-volatile.

134. The system of any one of claims 88 to 133, wherein the second widget is configured to provide the separator between the lithium rich intermediate electrode and the current collector substrate.

135. The system of claim 134, wherein the separator comprises a composite membrane comprising a lithium ion conductive polymer.

136. The system of any one of claims 88 to 135, wherein the separator comprises a lithium ion- selective membrane permitting lithium ions to selectively flow through.

137. The system of any one of claims 88 to 136, wherein the lithium ion-selective membrane comprises a single layer or multiple layers.

138. The system of any one of claims 88 to 137, wherein the lithium ion-selective membrane comprises glass fiber, polyester, polyethylene, polypropylene, polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), and a combination thereof.

139. The system of any one of claims 88 to 138, wherein the lithium ion-selective membrane comprises hydrophobic polymers.

140. The system of any one of claims 88 to 139, wherein the lithium ion-selective membrane comprises lithium-ion conductive channels.

141. The system of any one of claims 88 to 140, wherein a columbic efficiency of the system ranges from about 60% to about 100%.

142. The system of any one of claims 88 to 141, wherein a columbic efficiency of the system ranges from about 80% to about 100%.

143. The system of any one of claims 88 to 142, wherein the second widget is configured to produce a two-sided lithium metal electrode.

144. The system of any one of claims 88 to 143, wherein the lithium metal electrode is a batteryready electrode.

145. The system of any one of claims 88 to 144, wherein a surface roughness of the lithium metal electrode is less than about 3.0 pm.

146. The system of any one of claims 88 to 145, wherein a surface roughness of the lithium metal electrode is less than about 1.0 pm.

147. The system of any one of claims 88 to 146, wherein a purity of the lithium metal electrode is higher than about 98%.

148. The system of any one of claims 88 to 147, wherein a purity of the lithium metal electrode is higher than about 99.9%.

149. The system of any one of claims 88 to 148, wherein a deposition efficiency of the second widget is higher than about 95%.

150. The system of any one of claims 88 to 149, wherein a deposition efficiency of the second widget is higher than about 98%.

151. The system of any one of claims 88 to 150, wherein the lithium-rich intermediate electrode is delithiated at the second widget and returned to the first widget.

152. The system of any one of claims 88 to 151, wherein the lithium metal electrode is treated by refining or post processes.

153. The system of any one of claims 88 to 152, wherein the refining or post processes comprise cleaning, heating, calendaring, or applying pressure on the electrode.

154. The system of any one of claims 88 to 153, wherein the refining or post processes comprise applying heat to the electrode at a temperature below about 150°C.

155. The system of any one of claims 88 to 154, wherein the refining or post processes comprise applying pressure on the electrode at most 5 MPa.

156. The system of any one of claims 88 to 155, wherein the counter electrode, the intermediate electrode, and / or the current collector substrate are in a roll form.

157. The system of any one of claims 88 to 156, wherein the second widget further comprises a roll-to-roll production part.

158. The system of any one of claims 88 to 157, wherein the system is used for a scale-up production.

159. The system of any one of claims 88 to 158, wherein the system is configured to repeatedly produce a lithium metal electrode from one lithium rich intermediate electrode.

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