Electrochemical cell having a high-viscosity semi-solid electrode and method for manufacturing the same

Abstract

The embodiments described in this book relate to the recycling of electrodes and electrochemical cell materials. By recycling electrode materials, both the cost of the cryogen and the material itself can be significantly saved. The separation processes described in this book include centrifugation, sedimentation separation, flocculant separation, flotation, hydrocyclone, vibratory screening, air classification, and magnetic separation. In some embodiments, the methods described in this book can include any combination of flotation, air classification, and magnetic separation. In some embodiments, the electrolyte can be separated from the active material and / or the conductive material via drying, subcritical or supercritical carbon dioxide extraction, solvent mass extraction (e.g., using a non-aqueous or aqueous solvent), and / or freeze-drying. By applying these separation processes, high-purity raw material products can be separated. These products can be reused or sold to third parties. The processes described herein can be scaled up to large-scale cell production facilities.

Description

Technical Field

[0001] Cross - Reference to Related Applications This application claims priority to U.S. Provisional Patent Application No. 63 / 354,056, filed on June 21, 2022, titled "Electrochemical Cells with High - Viscosity Semi - Solid Electrodes, and Methods of Making the Same", the disclosure of which is hereby incorporated by reference in its entirety.

[0002] The embodiments described herein relate to high - viscosity semi - solid electrodes and methods of making the same.

Background Art

[0003] In the manufacture of electrochemical cells, an electrode can be coated on a current collector, and then an electrolyte can be added. Coating the current collector and adding the electrolyte are often performed in separate steps. This manufacturing process can limit the achievable electrode thickness and electrolyte selection. Semi - solid electrodes can be manufactured using an active material, a conductive material, and an electrolyte. The active material, conductive material, and electrolyte can be cast together as a semi - solid electrode. Semi - solid electrodes can be manufactured binder - free, thereby making it less likely to limit the movement of electroactive species. However, thick semi - solid electrodes are often inhibited by ion transport limitations. The reduction of lithium ions during charging or discharging can be a problem, especially during rapid charging or rapid discharging. These problems can be mitigated by improving ion transport.

Summary of the Invention

Means for Solving the Problems

[0004] The embodiments described herein relate to a method of manufacturing a semi - solid electrode. In some aspects, the method includes combining an active material with a conductive material and a non - aqueous liquid electrolyte to form a semi - solid anode, where the non - aqueous liquid electrolyte is at least about 2,000 mol / m 3is the salt concentration, a semi-solid anode is disposed on the anode current collector, the semi-solid anode has a thickness of at least about 150 μm, a cathode is disposed on the cathode current collector, the first surface of the separator is wetted with a non-aqueous liquid electrolyte, the first surface of the separator is coated with a carbon film, and the cathode is disposed on the anode with the separator sandwiched therebetween such that the first surface of the separator contacts the semi-solid anode to form an electrochemical cell. In some embodiments, the method may further include charging and discharging the electrochemical cell while the electrochemical cell is oriented such that the thickness of the anode is in line with the direction of gravity. In some embodiments, the non-aqueous liquid electrolyte has a salt concentration of at least about 3,000 mol / m 3 and can have. In some embodiments, the carbon film can include hard carbon. In some embodiments, the discharge is at a rate of at least about 1.5C. BRIEF DESCRIPTION OF THE DRAWINGS

[0005]

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DETAILED DESCRIPTION OF THE INVENTION

[0006] The embodiments described herein relate to high-viscosity semi-solid electrodes and methods for manufacturing the same. The semi-solid electrodes described herein can be made thicker (e.g., greater than 100 μm, up to 2,000 μm or more), (ii) with a higher loading of active material, and (iii) by a simplified manufacturing process that utilizes less equipment, due to (i) a decrease in the degree of bending and an increase in electronic conductivity of the semi-solid electrode. These relatively thick semi-solid electrodes reduce the volume, mass, and cost contribution of the inactive components to the active components, thereby enhancing the commercial attractiveness of the batteries manufactured using the semi-solid electrodes. In some embodiments, the semi-solid electrodes described herein are binderless and / or do not use binders used in conventional battery manufacturing. Instead, the volume of the electrode that is normally occupied by a binder in a conventional electrode is here occupied by the following: 1) electrolyte. It has the effect of reducing the degree of bending and increasing the total amount of salts available for ion diffusion, thereby counteracting the salt depletion effect characteristic of thick conventional electrodes when used at high rates. 2) active material. It has the effect of increasing the charge capacity of the battery. Or 3) conductive additive. It has the effect of increasing the electronic conductivity of the electrode, thereby counteracting the high internal impedance of thick conventional electrodes. The decrease in the degree of bending and the increase in electronic conductivity of the semi-solid electrodes described herein result in excellent rate characteristics and charge capacity of the electrochemical cells formed from the semi-solid electrodes. Since the semi-solid electrodes described herein can be made substantially thicker than conventional electrodes, the ratio of the active material (i.e., the semi-solid anode and / or cathode) to the inactive material (i.e., the current collector and separator) can be made much higher in a battery formed from an electrochemical cell stack including the semi-solid electrodes than in a similar battery formed from an electrochemical cell stack including conventional electrodes. As a result, the overall charge capacity and energy density of the batteries including the semi-solid electrodes described herein are substantially increased.

[0007] In some embodiments, the electrode materials described herein can be a flowable semi-solid or condensed liquid composition. In some embodiments, the electrode materials described herein can be binderless or substantially binder-free. A flowable semi-solid electrode can include a suspension of electrochemically active materials (cathode or anode particles or particulate), and optionally an electronically conductive material (e.g., carbon) in a non-aqueous liquid electrolyte. Stated another way, the active electrode particles and the conductive particles are co-suspended in the electrolyte to form a semi-solid electrode. Examples of battery architectures utilizing semi-solid suspensions are described in International Patent Publication No. WO2012 / 024499, entitled “Stationary, Fluid Redox Electrode,” and International Patent Publication No. WO2012 / 088442, entitled “Semi-Solid Filled Battery and Method of Manufacture.” The entire disclosures of these documents are incorporated herein by reference.

[0008] The power of thick electrodes is often limited by ion transport. Depletion of lithium ions during charging or discharging is a significant problem, especially in cells during rapid charging (e.g., at least 1C) or rapid discharging (e.g., at least 1C). High concentrations of electrolyte salts can mitigate lithium ion depletion. However, the long ion transport paths in thick electrodes can limit the rate capability of electrochemical cells with thick semi-solid electrodes. With respect to rate capability, ion transport has conventionally been thought to be dominated by electrophoresis and diffusion. Electrophoresis is the transport of ions driven by a voltage gradient. Diffusion is the transport of ions and species driven by a concentration gradient.

[0009] In some cases, the lithium ion transport and output of a cell with a semi-solid electrode can be facilitated by convection or bulk transport driven by a density gradient. Convection can be introduced into a thick semi-solid electrode using an electrolyte with a high salt concentration. A thick electrode using a high-concentration electrolyte can create a large concentration gradient in the electrolyte throughout the electrochemical cell during charge and discharge. This introduces a large density gradient, resulting in effective convective transport. Introducing an electrolyte with a high salt concentration can also increase the viscosity of the semi-solid electrode and the electrolyte therein, and potentially increase ion transport within the semi-solid electrode.

[0010] However, there are limits to the wettability of semi-solid electrodes. In other words, a semi-solid electrode with a high viscosity may have problems in contact with a separator and / or a current collector. Wetting the separator with an electrolyte solution promotes this contact. Contact and ion transfer can also be promoted by coating the separator and / or current collector with a carbon-containing material.

[0011] Cells using semi-solid electrodes and concentrated electrolytes have shown higher rate performance. Gravity and density gradients can be used to induce convective bulk transport. The density of the electrolyte can be caused by a temperature difference, the structure of the electrode material, and / or an electrolyte additive. The driving force causing bulk transport is not limited to gravity. In some embodiments, bulk transport may be caused by the application of a magnetic field, a temperature gradient, and / or a centrifugal force.

[0012] As used in this specification and the appended claims, the singular forms "a," "an," and "the" include plural referents unless the context clearly dictates otherwise. Thus, for example, the term "member" is intended to mean a single member or a combination of members, and the term "material" is intended to mean one or more materials, or a combination thereof.

[0013] When the term "substantially" is used in connection with "cylindrical", "linear", and / or other geometric relationships, it is intended to convey that the structure so defined is nominally cylindrical, linear, etc. As an example, a portion of a support member described as "substantially linear" is intended to convey that while linearity of that portion is desirable, some non-linearity may occur in the "substantially linear" portion. Such non-linearity can arise from manufacturing tolerances, or other practical considerations (such as pressure or force applied to the support member, etc.). Thus, a geometric structure modified by the term "substantially" includes such geometric characteristics within a plus or minus 5% tolerance of the described geometric structure. For example, a "substantially linear" portion is a portion that defines an axis or centerline within plus or minus 5% of being linear.

[0014] As used herein, the terms "set" and "plurality" may refer to a singular feature with a plurality of characteristics, or a plurality of parts. For example, when referring to a set of electrodes, the set of electrodes can be considered as one electrode with a plurality of parts, or the set of electrodes can be considered as a plurality of separate electrodes. Further, for example, when referring to a plurality of electrochemical cells, the plurality of electrochemical cells can be considered as a plurality of separate electrochemical cells, or one electrochemical cell with a plurality of parts. Thus, a set of parts or a plurality of parts may include a plurality of parts that are contiguous or discontinuous with each other. The plurality of particles or the plurality of substances can also be made from a plurality of articles that are separately manufactured and later joined to each other (e.g., by mixing, an adhesive, or any suitable method).

[0015] As used herein, the term "semi-solid" refers to a substance that is a mixture of a liquid phase and a solid phase, such as, for example, a particle suspension, a slurry, a colloidal suspension, an emulsion, a gel, or a micelle.

[0016] As used herein, the terms "activated carbon network" and "networked carbon" relate to the general qualitative state of an electrode. For example, an electrode comprising an activated carbon network (or networked carbon) is one in which the carbon particles within the electrode assume individual particle forms and arrangements that facilitate electrical contact and electrical conductivity between the particles and through the thickness and length of the electrode. Conversely, the terms "non-activated carbon network" and "non-networked carbon" relate to electrodes that exist as individual particle islands or multi-particle agglomerate islands where the carbon particles may not be sufficiently connected to provide adequate electrical conduction through the electrode.

[0017] As used herein, the terms "energy density" and "volume energy density" refer to the amount of energy (e.g., MJ) stored within an electrochemical cell per unit volume (e.g., L) of the materials (such as electrodes, separators, electrolytes, and current collectors) included for the operation of the electrochemical cell. Specifically, the materials used to package the electrochemical cell are excluded from the calculation of the volume energy density.

[0018] As used herein, the term "high-capacity material" or "high-capacity cathode material" refers to a material having an irreversible capacity greater than 300 mAh / g that can be incorporated within an electrode to facilitate the uptake of electroactive species. Examples include tin, tin alloys such as Sn-Fe, tin monoxide, silicon, silicon alloys such as Si-Co, silicon monoxide, aluminum, aluminum alloys, metal monoxides (such as CoO, FeO), or titanium oxide.

[0019] As used herein, the term "composite high-capacity electrode layer" refers to an electrode layer having both a high-capacity material and a conventional cathode material, such as a silicon graphite layer.

[0020] As used herein, the term "solid high-capacity electrode layer" refers to an electrode layer having a single solid-phase high-capacity material, such as sputtered silicon, tin, tin alloys such as Sn-Fe, tin monoxide, silicon, silicon alloys such as Si-Co, silicon monoxide, aluminum, aluminum alloys, metal monoxides (such as CoO, FeO), or titanium oxide.

[0021] As used herein, "density gradient" refers to the spatial variation of density at different depths. In other words, the amount of substance per unit volume changes from a first location to a second location.

[0022] Figure 1 is a block diagram of a method 10 for manufacturing a high-viscosity semi-solid electrode according to an embodiment. As shown, method 10 includes forming a semi-solid electrode by combining an active material with a conductive material and a non-aqueous liquid electrolyte in step 11, and disposing the semi-solid electrode on a first current collector in step 12. Method 10 optionally includes disposing a second electrode on a second current collector in step 13. Method 10 further includes wetting a first surface of the separator with a non-aqueous liquid electrolyte in step 14, and coating the first surface of the separator with a carbon coating in step 15. Method 10 includes disposing a second electrode on the semi-solid electrode with the separator interposed therebetween in step 16, and optionally horizontally charging and discharging the electrochemical cell in step 17.

[0023] Step 11 includes forming a semi-solid electrode by combining an active material, a conductive material, and a non-aqueous liquid electrolyte. In some embodiments, the semi-solid electrode can include an anode. In some embodiments, the semi-solid electrode can include a cathode. In some embodiments, the semi-solid electrode material can be pulverized and / or milled before mixing the semi-solid electrode material with a solvent. In some embodiments, the semi-solid electrode material can be pulverized and / or milled while mixing the semi-solid electrode material with a solvent. In some embodiments, the electrode slurry can be pulverized and / or crushed. In some embodiments, the semi-solid electrode material can be screened before mixing the semi-solid electrode material with a solvent. In some embodiments, the semi-solid electrode material can be screened while mixing the semi-solid electrode material with a solvent. Screening can separate large particles from the semi-solid electrode. In some embodiments, the electrode slurry can be screened. In some embodiments, screening can include employing a vibrating screen.

[0024] In some embodiments, the semi-solid electrode can include a cathode material. In some embodiments, the cathode material can include a tin metal alloy such as, for example, Sn-Co-C, Sn-Fe-C, Sn-Mg-C, or La-Ni-Sn alloy. In some embodiments, the cathode material can include an amorphous oxide such as, for example, SnO or SiO amorphous oxide. In some embodiments, the cathode material can include a glassy cathode such as, for example, Sn-Si-Al-B-O, Sn-Sb-S-O, SnO2-P2O5, or SnO-B2O3-P2O5-Al2O3 cathode. In some embodiments, the cathode material can include a metal oxide such as, for example, CoO, SnO2, V2O5. In some embodiments, the cathode material can include a metal nitride such as, for example, Li3N or Li2.6CoO.4N. In some embodiments, the cathode material can include a cathode active material selected from lithium metal, carbon, lithium intercalated carbon, lithium nitride, lithium alloy, and silicon, bismuth, boron, gallium, indium, zinc, tin, antimony, aluminum, titanium oxide, molybdenum, germanium, manganese, niobium, vanadium, tantalum, gold, platinum, iron, copper, chromium, nickel, cobalt, zirconium, yttrium, molybdenum oxide, germanium oxide, silicon oxide, silicon carbide, other high-capacity materials or their alloys, and any combination thereof. In some embodiments, the cathode active material can include silicon and / or its alloy. In some embodiments, the cathode active material can include tin and / or its alloy.

[0025] In some embodiments, the semi-solid electrode can include an anode material. In some embodiments, the anode material can include α-NaFeO2 (so-called "layered compound") or those having an orthorhombic-LiMnO2 structure type, or derivatives thereof with different crystal symmetries, atomic arrangements, or partial substitutions of metals or oxygen, including the general ordered rock salt compound LiMO2 group. M includes at least one first transition metal, but may also include non-transition metals including, but not limited to, Al, Ca, Mg, Zr. Examples of such compounds include LiFePO4 (LFP), LiCoO2, Mg-doped LiCoO2, LiNiO2, Li(Ni, Co, Al)O2 (known as "NCA"), Li(Ni, Mn, Co)O2 (known as "NMC"), etc. In some embodiments, the anode material can include spinel structures such as LiMn2O4 and its derivatives, so-called "layered spinel nanocomposites", which structures include nanoscopic regions having ordered rock salt and spinel order, olivine LiMPO4 and its derivatives where M includes one or more of Mn, Fe, Co, or Ni, partially fluorinated compounds such as LiVPO4F, other "polyanion" compounds as described below, and vanadium oxides V 11 including vanadium oxide V x O y can be included. In some embodiments, the anode material can include transition metal polyanion compounds. In some embodiments, the anode material can include alkali metal transition metal oxides or phosphates. For example, the compound has the composition A x (M′ 1-a M″ a ) y (XD4) z , A x (M′ 1-a M″ a ) y (DXD4) z , or A x (M′ 1-a M″ a ) y (X2D7) z, having, the value obtained by adding the formal valence number(s) of M' multiplied by y(1 - a) times x and the formal valence number(s) of M'' multiplied by y(a) times is equal to z times the formal valence number of the XD4, X2D7, or DXD4 group. Or, the composition (A1 - a M'' a ) x M' y (XD4) z , (A1 - a M'' a ) x (M' y (DXD4)z(A1 - a M'' a ) a M' y (X2D7) z is a compound containing, having the formal valence number(s) of M'' multiplied by ax times (1 - a)x, and further the value obtained by adding the formal valence number(s) of M' multiplied by y times is equal to z times the formal valence number of the XD4, X2D7, or DXD4 group. In the compound, A is at least one of an alkali metal and hydrogen, M' is a first transition metal, X is at least one of phosphorus, sulfur, arsenic, molybdenum, and tungsten, M'' is any one of metals of Group HA, IIIA, IVA, VA, VIA, VIIA, VIIIA, IB, IIB, IIIB, IVB, VB, and VIB, and D is at least one of oxygen, nitrogen, carbon, and halogen. The positive electrode active material can be an olivine structure compound LiMPO4, M is one or more of V, Cr, Mn, Fe, Co, and Ni, and this compound is optionally potentially doped at the Li, M, and O sites. The deficiency at the Li site is compensated by the addition of a metal or metalloid, and the deficiency at the O site is compensated by the addition of a halogen. In some embodiments, the positive active material has an olivine structure and contains a thermally stable transition metal-doped lithium transition metal phosphate having the formula (Li 1-x Z x )MPO4, where M is one or more of V, Cr, Mn, Fe, Co, and Ni, Z is a non-alkali metal dopant such as one or more of Ti, Zr, Nb, Al, or Mg, and x ranges from 0.005 to 0.05.

[0026] In some embodiments, the conductive material can include activated carbon, hard carbon, soft carbon, Ketjen, carbon black, graphite carbon, carbon fiber, carbon microfiber, allotropes of carbon including vapor-grown carbon fiber (VGCF), fullerene-based carbon including "buckyballs", carbon nanotubes (CNT), multi-walled carbon nanotubes (MWNT), single-walled carbon nanotubes (SWNT), graphene sheets or aggregates of graphene sheets, and substances composed of fullerene-based fragments, or any combination thereof. In some embodiments, the active material, conductive material, and / or electrolyte solution can include any of the materials described in U.S. Patent No. 9,437,864, titled "Asymmetric Battery Having a Semi-solid Cathode and High Energy Density Anode", filed on March 10, 2014 (hereinafter, the "864 patent"), the disclosure of which is hereby incorporated by reference in its entirety.

[0027] In some embodiments, the non-aqueous liquid electrolyte can include an electrolyte solvent and an electrolyte salt. In some embodiments, the electrolyte solvent can include vinylene carbonate (VC), 1,3-propane sultone (PS), ethyl propionate (EP), 1,3-propanediol cyclic sulfate (PSA / TS), fluoroethylene carbonate (FEC), ethylene sulfite (ES), tris(2-ethylhexyl) phosphate (TOP), 1,3,2-dioxathiolane 2,2-dioxide (DTD), ethyl acetate (EA), maleic anhydride (MA), ethylene carbonate (EC), propylene carbonate (PC), dimethyl carbonate (DMC), ethyl methyl carbonate (EMC), or a combination thereof. In some embodiments, the electrolyte salt can include lithium bis(oxalato)borate (LiBOB), lithium hexafluorophosphate (LiPF6), lithium bis(fluorosulfonyl)imide (LiFSI), or any combination thereof.

[0028] In some embodiments, the concentration of the electrolyte salt in the electrolyte solution is at least about 1.5 M, at least about 2 M, at least about 2.5 M, at least about 3 M, at least about 3.5 M, at least about 4 M, at least about 4.5 M, at least about 5 M, at least about 5.5 M, at least about 6 M, at least about 6.5 M, at least about 7 M, at least about 7.5 M, at least about 8 M, at least about 8.5 M, at least about 9 M, or at least about 9.5 M. In some embodiments, the electrolyte salt has a concentration in the electrolyte solution of about 10 M or less, about 9.5 M or less, about 9 M or less, about 8.5 M or less, about 8 M or less, about 7.5 M or less, about 7 M or less, about 6.5 M or less, about 5 M or less, about 5.5 M or less, about 5 M or less, about 4.5 M, about 4 M or less, about 3.5 M or less, about 3 M or less, about 2.5 M or less, or about 2 M or less. Combinations of the above salt concentrations are also possible (e.g., at least about 1.5 M or more and less than about 10 M, or at least about 3 M or more and less than about 5 M), including all values and ranges therebetween. In some embodiments, the electrolyte salt can have a concentration in the electrolyte solution of about 1.5 M, about 2 M, about 2.5 M, about 3 M, about 3.5 M, about 4 M, about 4.5 M, about 5 M, about 5.5 M, about 6 M, about 6.5 M, about 7 M, about 7.5 M, about 8 M, about 8.5 M, about 9 M, about 9.5 M, or about 10 M.

[0029] In some embodiments, the electrolyte can include a single salt. In some embodiments, the electrolyte can include about 2, about 3, about 4, about 5, about 6, about 7, about 8, about 9, or about 10 salts, including all values and ranges therebetween. In some embodiments, the electrolyte salt can include LiFSi, LiPF6, or any combination thereof. For example, the electrolyte salt can include about 2 M of LiFSI. As an additional example, the electrolyte salt can include about 1.5 M LiPF6 including about 0.5 M of LiFSI.

[0030] In some embodiments, the electrolyte can include a single electrolyte solvent. In some embodiments, the electrolyte can include about 2, about 3, about 4, about 5, about 6, about 7, about 8, about 9, or about 10 electrolyte solvents, including all values and ranges therebetween. In some embodiments, the electrolyte solvent can include EC, PC, EMC, MA, or any combination thereof, and in any ratio. For example, the electrolyte solvent can include EC / PC / EMC in a ratio of about 2 parts (by weight) of EC, about 1 part of PC, and about 7 parts of EMC. As an additional example, the electrolyte solvent can include EC / PC / EMC / MA in a ratio of about 1 part of PC to about 2 parts of EC and about 4 parts of MA to about 3 parts of EMC.

[0031] In some embodiments, the electrolyte can include an additive or combination of additives. In some embodiments, the electrolyte can include about 0.1 wt%, about 0.2 wt%, about 0.3 wt%, about 0.4 wt%, about 0.5 wt%, about 0.6 wt%, about 0.7 wt%, about 0.8 wt%, about 0.9 wt%, about 1 wt%, about 1.5 wt%, about 2 wt%, about 2.5 wt%, about 3 wt%, about 3.5 wt%, about 4 wt%, about 4.5 wt%, about 5 wt%, about 5.5 wt%, about 6 wt%, about 6.5 wt%, about 7 wt%, about 7.5 wt%, about 8 wt%, about 8.5 wt%, about 9 wt%, about 9.5 wt%, or about 10 wt% (including all values and ranges therebetween). In some embodiments, the additive is VC, DTD, 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether (TTE), lithium difluoro(oxalato)borate (LiDFOB), FEC, tris(trimethylsilyl) phosphate (TMSP8), tris(2,2,2-trifluoroethyl) borate (TTFEB), 1,4-butanesultone (BuS), 1731460358672_0.2c02658 For example, the electrolyte can include about 0.5 wt% to about 2 wt% of VC, about 1 wt% to about 1.5 wt% of DTD, about 0.5 wt% to about 3 wt% of TTE, and about 0.5 wt% to about 1 wt% of LiDFOB. As an additional example, the electrolyte can include about 0.5 wt% to about 2 wt% of VC, about 1 wt% to about 1.5 wt% of DTD, about 0.5 wt% to about 3 wt% of TTE, about 0.5 wt% to about 1 wt% of LiDFOB, and about 0.1 wt% to about 1 wt% of FEC. As an additional example, the electrolyte can include about 0.5 wt% to about 2 wt% of VC, about 1 wt% to about 1.5 wt% of DTD, about 0.5 wt% to about 3 wt% of TTE, about 0.5 wt% to about 1 wt% of LiDFOB, and about 0.1 wt% to about 1 wt% of TMSP8. As an additional example, the electrolyte can include about 0.5 wt% to about 2 wt% of VC, about 1 wt% to about 1.5 wt% of DTD, and about 0.5 wt% to about 2 wt% of TTFEB. As an additional example, the electrolyte can include about 0.5 wt% to about 2 wt% of VC and about 0.5 wt% to about 1 wt% of BuS. As an additional example, the electrolyte can include about 0.5 wt% to about 2 wt% of VC and about 0.5 wt% to about 1 wt% of LiPO2F2. As an additional example, the electrolyte can include about 0.5 wt% to about 2 wt% of VC, about 0.5 wt% to about 1 wt% of BuS, and about 0.5 wt% to about 1 wt% of LiPO2F2.

[0032] In some embodiments, the active material, conductive material, and / or electrolyte solution can be combined via mixing, high-shear mixing, planetary mixing, centrifugal planetary mixing, sigma mixing, crack attenuation mixing (CAM) mixing, roller mixing, or any combination thereof. In some embodiments, the active material, conductive material, and / or electrolyte solution can be mixed together with a mixing index of at least about 0.8, at least about 0.85, at least about 0.9, at least about 0.95, or at least about 0.975 (including all values and ranges therebetween). In some embodiments, the active material, conductive material, and / or electrolyte solution can be combined via any of the mixing methods described in U.S. Patent Publication No. 2017 / 0162863, filed on September 15, 2016, and entitled “Electrochemical Slurry Compositions and Methods for Preparing the Same” (‘863 Publication), the entire disclosure of which is incorporated herein by reference.

[0033] Step 12 includes disposing a semi-solid electrode on a first current collector. In some embodiments, the semi-solid electrode can be dispensed and / or extruded via a sheet extrusion die, a profile sheet extrusion die, any nozzle, a single-screw extruder, a twin-screw extruder, or an injection molding die. In some embodiments, the semi-solid electrode can have a viscosity (at 25° C.) of at least about 100 Pa·s, at least about 150 Pa·s, at least about 200 Pa·s, at least about 250 Pa·s, at least about 300 Pa·s, at least about 350 Pa·s, at least about 400 Pa·s, at least about 450 Pa·s, at least about 500 Pa·s, at least about 550 Pa·s, at least about 600 Pa·s, at least about 650 Pa·s, at least about 700 Pa·s, at least about 750 Pa·s, at least about 800 Pa·s, at least about 850 Pa·s, at least about 900 Pa·s, or at least about 950 Pa·s. In some embodiments, the semi-solid electrode can have a viscosity of about 1,000 Pa·s or less, about 950 Pa·s or less, about 900 Pa·s or less, about 850 Pa·s or less, about 800 Pa·s or less, about 750 Pa·s or less, about 700 Pa·s or less, about 650 Pa·s or less, about 600 Pa·s or less, about 550 Pa·s or less, about 500 Pa·s or less, about 450 Pa·s or less, about 400 Pa·s or less, about 350 Pa·s or less, about 300 Pa·s or less, about 250 Pa·s or less, about 200 Pa·s or less, or about 950 Pa·s or less. Combinations of the above viscosities are also possible (e.g., at least about 100 Pa·s or more and about 1,000 Pa·s or less, or at least about 300 Pa·s or more and about 600 Pa·s or less), including all values and ranges therebetween. In some embodiments, the semi-solid electrode can have a viscosity of about 100 Pa·s, about 150 Pa·s, about 200 Pa·s, about 250 Pa·s, about 300 Pa·s, about 350 Pa·s, about 400 Pa·s, about 450 Pa·s, about 500 Pa·s, about 550 Pa·s, about 600 Pa·s, about 650 Pa·s, about 700 Pa·s, about 750 Pa·s, about 800 Pa·s, about 850 Pa·s, about 900 Pa·s, about 950 Pa·s, or about 1,000 Pa·s.

[0034] When a semi-solid electrode is disposed on a first current collector, the semi-solid electrode has a thickness. In some embodiments, the thickness of the semi-solid electrode is at least about 100 μm, at least about 150 μm, at least about 200 μm, at least about 250 μm, at least about 300 μm, at least about 350 μm, at least about 400 μm, at least about 450 μm, at least about 500 μm, at least about 550 μm, at least about 600 μm, at least about 650 μm, at least about 700 μm, at least about 750 μm, at least about 800 μm, at least about 850 μm, at least about 900 μm, at least about 950 μm, at least about 1,000 μm, at least about 1,050 μm, at least about 1,100 μm, at least about 1,150 μm, at least about 1,200 μm, at least about 1,250 μm, at least about 1,300 μm, at least about 1,350 μm, at least about 1,400 μm, at least about 1,450 μm, at least about 1,500 μm, at least about 1,550 μm, at least about 1,600 μm, at least about 1,650 μm, at least about 1,700 μm, at least about 1,750 μm, at least about 1,800 μm, at least about 1,850 μm, at least about 1,900 μm, or at least about 1,950 μm. In some embodiments, the thickness of the semi-solid electrode is about 2,000 μm or less, about 1,950 μm or less, about 1,900 μm or less, about 1,850 μm or less, about 1,800 μm or less, about 1,750 μm or less, about 1,700 μm or less, about 1,650 μm or less, about 1,600 μm or less, about 1,550 μm or less, about 1,500 μm or less, about 1,450 μm or less, about 1,400 μm or less, about 1,350 μm or less, about 1,300 μm or less, about 1,250 μm or less, about 1,200 μm or less, about 1,150 μm or less, about 1,100 μm or less, about 1,050 μm or less, about 1,000 μm or less, about 950 μm or less, about 900 μm or less, about 850 μm or less, about 800 μm or less, about 750 μm or less, about 700 μm or less, about 650 μm or less, about 600 μm or less, about 550 μm or less, about 500 μm or less, about 450 μm or less, about 400 μm or less, about 350 μm or less, about 300 μm or less, about 250 μm or less, about 200 μm or less, or about 150 μm or less.The above thickness combinations are also possible (e.g., at least about 100 μm and about 2,000 μm or less, or at least about 300 μm and about 1,000 μm or less), including all values and ranges therebetween. In some embodiments, the thickness of the semi-solid electrode can be about 100 μm, about 150 μm, about 200 μm, about 250 μm, about 300 μm, about 350 μm, about 400 μm, about 450 μm, about 500 μm, about 550 μm, about 600 μm, about 650 μm, about 700 μm, about 750 μm, about 800 μm, about 850 μm, about 900 μm, about 950 μm, about 1,000 μm, about 1,050 μm, about 1,100 μm, about 1,150 μm, about 1,200 μm, about 1,250 μm, about 1,300 μm, about 1,350 μm, about 1,400 μm, about 1,450 μm, about 1,500 μm, about 1,550 μm, about 1,600 μm, about 1,650 μm, about 1,700 μm, about 1,750 μm, about 1,800 μm, about 1,850 μm, about 1,900 μm, about 1,950 μm, or about 2,000 μm.

[0035] In step 13, method 10 optionally includes disposing a second electrode on a second current collector. In some embodiments, the second electrode can include a cathode. In some embodiments, the second electrode can include an anode. In some embodiments, the second electrode can include a semi-solid electrode. In some embodiments, the second electrode can include a solid or "conventional" electrode.

[0036] When the second electrode is disposed on the second current collector, the second electrode has a thickness. In some embodiments, the second electrode can have a thickness of at least about 20 μm, at least about 30 μm, at least about 40 μm, at least about 50 μm, at least about 60 μm, at least about 70 μm, at least about 80 μm, or at least about 90 μm. In some embodiments, the second electrode can have a thickness of about 100 μm or less, about 90 μm or less, about 80 μm or less, about 70 μm or less, about 60 μm or less, about 50 μm or less, about 40 μm or less, or about 30 μm or less. Combinations of the above thicknesses of the second electrode are also possible (e.g., at least about 20 μm or more and about 100 μm or less, or at least about 40 μm or more and about 80 μm or less), including all values and ranges therebetween. In some embodiments, the second electrode can have a thickness of about 20 μm, about 30 μm, about 40 μm, about 50 μm, about 60 μm, about 70 μm, about 80 μm, about 90 μm, or about 100 μm.

[0037] In step 14, method 10 includes wetting a first surface of the separator with a non-aqueous liquid electrolyte. In some embodiments, the wetting can be performed via spraying, brush coating, injection (e.g., by syringe), inkjet printing, slot die dropping, coating, or any other suitable application means. In some embodiments, the non-aqueous liquid electrolyte coated on the first surface of the separator can have the same concentration or a substantially similar concentration as the non-aqueous liquid electrolyte included in the semi-solid electrode. In some embodiments, both sides of the separator can be coated with the non-aqueous liquid electrolyte.

[0038] Step 15 includes coating the first surface of the separator with carbon. In some embodiments, the carbon coating can include hard carbon, disordered carbon, graphite, graphite-like carbon or non-graphite carbon, amorphous carbon, mesocarbon, microbeads, soft carbon, activated carbon, a graphite-like hard carbon mixture, or any combination thereof. In some embodiments, the carbon coating can include a crystalline portion and an amorphous portion. In some embodiments, the carbon coating can include activated carbon, ketjen, carbon nanotubes, carbon fibers, or any combination thereof. In some embodiments, the non-aqueous electrolyte can facilitate the attachment of the carbon coating to the first surface of the carbon coating.

[0039] Step 16 is optional and includes disposing a second electrode on the semi-solid electrode with a separator interposed therebetween between the second electrode and the semi-solid electrode. This forms an electrochemical cell. The first surface of the separator (i.e., the surface of the separator coated with the non-aqueous liquid electrolyte solution and the carbon coating) contacts the semi-solid electrode. The non-aqueous liquid electrolyte solution and the carbon coating facilitate the electrochemical contact between the semi-solid electrode and the separator.

[0040] Step 17 is optional and includes charging and discharging the electrochemical cell in a horizontal direction. In other words, the electrochemical cell is charged and discharged with the electrodes oriented horizontally such that gravity acts in the thickness direction of the electrodes. Gravity creates a density gradient and a salt concentration gradient within the highly viscous semi-solid electrode. In some embodiments, the density gradient can be created via a magnetic field. In some embodiments, the density gradient can be created by heating the semi-solid electrode. In some embodiments, the density gradient can be created by centrifugal force. In some embodiments, while operating the electrochemical cell, the electrochemical cell can be rotated about a central axis. In some embodiments, a plurality of electrochemical cells can be rotated about a central axis to create a density gradient.

[0041] In some embodiments, the electrochemical cell can be charged at a rate of at least about 1 C, at least about 1.5 C, at least about 2 C, at least about 2.5 C, at least about 3 C, at least about 3.5 C, at least about 4 C, at least about 4.5 C, at least about 5 C, at least about 5.5 C, at least about 6 C, at least about 6.5 C, at least about 7 C, at least about 7.5 C, at least about 8 C, at least about 8.5 C, at least about 9 C, at least about 9.5 C, or at least about 10 C (including all values and ranges therebetween). In some embodiments, the electrochemical cell can be discharged at a rate of at least about 1 C, at least about 1.5 C, at least about 2 C, at least about 2.5 C, at least about 3 C, at least about 3.5 C, at least about 4 C, at least about 4.5 C, at least about 5 C, at least about 5.5 C, at least about 6 C, at least about 6.5 C, at least about 7 C, at least about 7.5 C, at least about 8 C, at least about 8.5 C, at least about 9 C, at least about 9.5 C, or at least about 10 C (including all values and ranges therebetween).

[0042] FIG. 2 is a block diagram of an electrochemical cell 200 according to one embodiment. As shown, the electrochemical cell 200 includes a cathode 210 disposed on a cathode current collector 220, an anode 230 disposed on an anode current collector 240, and a separator 250 disposed between the cathode 210 and the anode 230. Optionally, a carbon coating 260 is disposed between the anode 230 and the separator 250.

[0043] The cathode 210 includes a cathode active material. In some embodiments, the cathode 210 can include any of the above cathode materials. In some embodiments, the cathode 210 can include a semi-solid cathode. In some embodiments, the cathode 210 has at least about 500 mol / m 3 , at least about 1,000 mol / m 3 , at least about 1,500 mol / m 3 , at least about 2,000 mol / m 3 , at least about 2,100 mol / m 3, at least about 2,200 mol / m 3 , at least about 2,300 mol / m 3 , at least about 2,400 mol / m 3 , at least about 2,500 mol / m 3 , at least about 3,000 mol / m 3 , at least about 3,500 mol / m 3 , at least about 4,000 mol / m 3 , at least about 4,500 mol / m 3 , at least about 5,000 mol / m 3 , at least about 5,500 mol / m 3 , at least about 6,000 mol / m 3 , at least about 6,500 mol / m 3 , at least about 7,000 mol / m 3 , at least about 7,500 mol / m 3 , at least about 8,000 mol / m 3 , at least about 8,500 mol / m 3 , at least about 9,000 mol / m 3 , or at least about 9,500 mol / m 3 and can have an electrolyte salt concentration. In some embodiments, the cathode 210 is about 10,000 mol / m 3 or less, about 9,500 mol / m 3 or less, about 9,000 mol / m 3 or less, about 8,500 mol / m 3 or less, about 8,000 mol / m 3 or less, about 7,500 mol / m 3 or less, about 7,000 mol / m 3 or less, about 6,500 mol / m 3 or less, about 6,000 mol / m 3 or less, about 5,500 mol / m 3 , about 5,000 mol / m 3 or less, about 4,500 mol / m 3 or less, about 4,000 mol / m 3 or less, about 3,500 mol / m 3 or less, about 3,000 mol / m 3 or less, about 2,500 mol / m3 Less than or about 2,400 mol / m 3 Less than or about 2,300 mol / m 3 Less than or about 2,200 mol / m 3 Less than or about 2,100 mol / m 3 Less than or about 2,000 mol / m 3 Less than or about 1,500 mol / m 3 Less than or about 1,000 mol / m 3 It can have the following electrolyte salt concentrations. Combinations of the above electrolyte salt concentrations in the cathode 210 are also possible (for example, at least about 500 mol / m 3 and about 10,000 mol / m 3 Less than or at least about 2,000 mol / m 3 and about 5,000 mol / m 3 Less than or the like), including all values and ranges therebetween. In some embodiments, the cathode 210 is about 500 mol / m 3 , about 1,000 mol / m 3 , about 1,500 mol / m 3 , about 2,000 mol / m 3 , about 2,100 mol / m 3 , about 2,200 mol / m 3 , about 2,300 mol / m 3 , about 2,400 mol / m 3 , about 2,500 mol / m 3 , about 3,000 mol / m 3 About 3,500 mol / m 3 , about 4,000 mol / m 3 , about 4,500 mol / m 3 , about 5,000 mol / m 3 , about 5,500 mol / m 3 , about 6,000 mol / m 3 , about 6,500 mol / m 3 , about 7,000 mol / m 3 , about 7,500 mol / m 3 , about 8,000 mol / m 3 , about 8,500 mol / m 3 , about 9,000 mol / m 3 , about 9,500 mol / m 3 , or about 10,000 mol / m3 can have an electrolyte salt concentration. In some embodiments, the electrolyte salt concentration can be measured directly. In some embodiments, the electrolyte salt concentration can be estimated via simulations based on finite element modeling.

[0044] In some embodiments, the cathode 210 can have an electrolyte salt concentration gradient along the thickness of the cathode 210. In some embodiments, the concentration gradient can exist while the electrochemical cell 200 is charging. In some embodiments, the concentration gradient can exist while the electrochemical cell 200 is discharging. In some embodiments, the concentration gradient can exist while the electrochemical cell 200 is in a resting state. In some embodiments, the cathode 210 is at least about 1×10 7 mol / m 4 , at least about 1.1×10 7 mol / m 4 , at least about 1.2×10 7 mol / m 4 , at least about 1.3×10 7 mol / m 4 , at least about 1.4×10 7 mol / m 4 , at least about 1.5×10 7 mol / m 4 , at least about 1.6×10 7 mol / m 4 , at least about 1.7×10 7 mol / m 4 , at least about 1.8×10 7 mol / m 4 , at least about 1.9×10 7 mol / m 4 , at least about 2×10 7 mol / m 4 , at least about 2.1×10 7 mol / m 4 , at least about 2.2×10 7 mol / m 4 , at least about 2.3×10 7 mol / m 4 , at least about 2.4×10 7mol / m 4 and at least about 2.5×10 7 mol / m 4 and at least about 2.6×10 7 mol / m 4 and at least about 2.7×10 7 mol / m 4 and at least about 2.8×10 7 mol / m 4、 and at least about 2.9×10 7 mol / m 4 and at least about 3×10 7 mol / m 4 and at least about 3.1×10 7 mol / m 4 and at least about 3.2×10 7 mol / m 4 and at least about 3.3×10 7 mol / m 4 and at least about 3.4×10 7 mol / m 4 and at least about 3.5×10 7 mol / m 4 and at least about 3.6×10 7 mol / m 4 and at least about 3.7×10 7 mol / m 4 and at least about 3.8×10 7 mol / m 4 and at least about 3.9×10 7 mol / m 4 and at least about 4×10 7 mol / m 4 and at least about 4.1×10 7 mol / m 4 and at least about 4.2×10 7 mol / m 4 and at least about 4.3×10 7 mol / m 4 and at least about 4.4×10 7 mol / m 4 and at least about 4.5×10 7 mol / m 4 and at least about 4.6×10 7 mol / m 4 and at least about 4.7×107 mol / m 4 and at least about 4.8×10 7 mol / m 4 and at least about 4.9×10 7 mol / m 4 and can have an average electrolyte salt concentration gradient. In some embodiments, the cathode 210 is about 5×10 7 mol / m 4 or less, about 4.9×10 7 mol / m 4 or less, about 4.8×10 7 mol / m 4 or less, about 4.7×10 7 mol / m 4 or less, about 4.6×10 7 mol / m 4 or less, about 4.5×10 7 mol / m 4 or less, about 4.4×10 7 mol / m 4 or less, about 4.3x10 7 mol / m 4 or less, about 4.2x10 7 mol / m 4 or less, about 4.1x10 7 mol / m 4 or less, about 4x10 7 mol / m 4 or less, about 3.9x10 7 mol / m 4 or less, about 3.8x10 7 mol / m 4 or less, about 3.7×10 7 mol / m 4 or less, about 3.6×10 7 mol / m 4 or less, about 3.5×10 7 mol / m 4 or less, about 3.4×10 7 mol / m 4 or less, about 3.3×10 7 mol / m 4 or less, about 3.2x10 7 mol / m 4 or less, about 3.1x10 7 mol / m 4 or less, about 3x10 7 mol / m4 The following is about 2.9x10 7 mol / m 4 The following is about 2.8x10 7 mol / m 4 The following is about 2.7x10 7 mol / m 4 The following is about 2.6x10 7 mol / m 4 The following is about 2.5x10 7 mol / m 4 The following is about 2.4x10 7 mol / m 4 The following is about 2.3x10 7 mol / m 4 The following is about 2.2x10 7 mol / m 4 The following is about 2.1×10 7 mol / m 4 The following is about 2×10 7 mol / m 4 The following is about 1.9×10 7 mol / m 4 The following is about 1.8×10 7 mol / m 4 The following is about 1.7×10 7 mol / m 4 The following is about 1.6×10 7 mol / m 4 The following is about 1.5×10 7 mol / m 4 The following is about 1.4×10 7 mol / m 4 The following is about 1.3×10 7 mol / m 4 The following is about 1.2×10 7 mol / m 4 The following, or about 1.1×10 7 mol / m 4 It can have the following average electrolyte salt concentration gradients.

[0045] Combinations of the above average electrolyte salt concentration gradients are also possible (for example, at least about 1×10 7 mol / m 4 or more and about 5×10 7 mol / m 4 or less, or at least about 2 mol / m 4about 4 mol / m 4 or less), including all values and ranges therebetween. In some embodiments, the cathode 210 is about 1.0×10 7 mol / m 4 , about 1.1×10 7 mol / m 4 , about 1.2×10 7 mol / m 4 , about 1.3×10 7 mol / m 4 , about 1.4×10 7 mol / m 4 , about 1.5×10 7 mol / m 4 , about 1.6×10 7 mol / m 4 , about 1.7×10 7 mol / m 4 , about 1.8×10 7 mol / m 4 , about 1.9×10 7 mol / m 4 , about 2.0×10 7 mol / m 4 , about 2.1×10 7 mol / m 4 , about 2.2×10 7 mol / m 4 , about 2.3×10 7 mol / m 4 , about 2.4×10 7 mol / m 4 , about 2.5×10 7 mol / m 4 , about 2.6×10 7 mol / m 4 , about 2.7×10 7 mol / m 4 , about 2.8×10 7 mol / m 4 , about 2.9×10 7 mol / m 4 , about 3.0×10 7 mol / m 4 , about 3.1×10 7 mol / m 4 , about 3.2×10 7 mol / m 4 , about 3.3×10 7 mol / m 4, about 3.4×10 7 mol / m 4 , about 3.5×10 7 mol / m 4 , about 3.6×10 7 mol / m 4 , about 3.7×10 7 mol / m 4 , about 3.8×10 7 mol / m 4 , about 3.9×10 7 mol / m 4 , about 4.0×10 7 mol / m 4 , about 4.1×10 7 mol / m 4 , about 4.2×10 7 mol / m 4 , about 4.3×10 7 mol / m 4 , about 4.4×10 7 mol / m 4 , about 4.5×10 7 mol / m 4 , about 4.6×10 7 mol / m 4 , about 4.7×10 7 mol / m 4 , about 4.8×10 7 mol / m 4 , about 4.9×10 7 mol / m 4 , or about 5.0×10 7 mol / m 4 and can have an average electrolyte salt concentration gradient.

[0046] In some embodiments, the cathode 210 can have a density gradient. In some embodiments, the density gradient can exist while the electrochemical cell 200 is charging. In some embodiments, the density gradient can exist while the electrochemical cell 200 is discharging. In some embodiments, the density gradient can exist while the electrochemical cell 200 is resting. In some embodiments, the cathode 210 is at least about 1×10 5 kg / m 4 , at least about 2×10 5 kg / m 4, at least about 3×10 5 kg / m 4 , at least about 4×10 5 kg / m 4 , at least about 5×10 5 kg / m 4 , at least about 6×10 5 kg / m 4 , at least about 7×10 5 kg / m 4 , at least about 8×10 5 kg / m 4 , at least about 9×10 5 kg / m 4 , at least about 1×10 6 kg / m 4 , at least about 2×10 6 kg / m 4 , at least about 3×10 6 kg / m 4 , at least about 4×10 6 kg / m 4 , at least about 5×10 6 kg / m 4 , at least about 6×10 6 kg / m 4 , at least about 7×10 6 kg / m 4 , at least about 8×10 6 kg / m 4 , at least about 9×10 6 kg / m 4 , at least about 1×10 7 kg / m 4 , at least about 2×10 7 kg / m 4 , at least about 3×10 7 kg / m 4 , at least about 4×10 7 kg / m 4 , at least about 5×10 7 kg / m 4 , at least about 6×10 7 kg / m 4 , at least about 7×10 7 kg / m 4 , at least about 8×10 7 kg / m 4 , at least about 9×107 kg / m 4 and at least about 1×10 8 kg / m 4 and at least about 2×10 8 kg / m 4 and at least about 3×10 8 kg / m 4 and at least about 4×10 8 kg / m 4 and at least about 5×10 8 kg / m 4 and at least about 6×10 8 kg / m 4 and at least about 7×10 8 kg / m 4 and at least about 8×10 8 kg / m 4 or at least about 9×10 8 kg / m 4 average density gradient. In some embodiments, the cathode 210 is about 1×10 9 kg / m 4 or less, about 9×10 8 kg / m 4 or less, about 8×10 8 kg / m 4 or less, about 7×10 8 kg / m 4 or less, about 6×10 8 kg / m 4 or less, about 5×10 8 kg / m 4 or less, about 4×10 8 kg / m 4 about 3×10 8 kg / m 4 or less, about 2×10 8 kg / m 4 or less, about 1×10 8 kg / m 4 or less, about 9×10 7 kg / m 4 or less, about 8×10 7 kg / m 4 or less, about 7×10 7 kg / m 4 or less, about 6×10 7 kg / m 4 or less, about 5×10 7 kg / m 4The following, about 4×10 7 kg / m 4 The following, about 3×10 7 kg / m 4 The following, about 2×10 7 kg / m 4 The following, about 1×10 7 kg / m 4 The following, about 9×10 6 kg / m 4 The following, about 8×10 6 kg / m 4 The following, about 7×10 6 kg / m 4 The following, about 6×10 6 kg / m 4 The following, about 5×10 6 kg / m 4 The following, about 4×10 6 kg / m 4 The following, about 3×10 6 kg / m 4 The following, about 2×10 6 kg / m 4 The following, about 1×10 6 kg / m 4 The following, about 9×10 5 kg / m 4 The following, about 8×10 5 kg / m 4 The following, about 7×10 5 kg / m 4 The following, about 6×10 5 kg / m 4 The following, about 5×10 5 kg / m 4 The following, about 4×10 5 kg / m 4 The following, about 3×10 5 kg / m 4 The following, or about 2×10 5 kg / m 4 can have the following average concentration gradient.

[0047] Combinations of the above average concentration gradients are also possible (for example, at least about 1×10 5 kg / m 4 , about 1×10 9 kg / m 4 The following, or at least about 1×10 6 kg / m4 , about 1×10 8 kg / m 4 or less), including all values and ranges therebetween. In some embodiments, the cathode 210 is about 1×10 5 kg / m 4 , about 2×10 5 kg / m 4 , about 3×10 5 kg / m 4 , about 4×10 5 kg / m 4 , about 5×10 5 kg / m 4 , about 6×10 5 kg / m 4 , about 7×10 5 kg / m 4 , about 8×10 5 kg / m 4 , about 9×10 5 kg / m 4 , about 1×10 6 kg / m 4 , about 2×10 6 kg / m 4 , about 3×10 6 kg / m 4 , about 4×10 6 kg / m 4 , about 5×10 6 kg / m 4 , about 6×10 6 kg / m 4 , about 7×10 6 kg / m 4 , about 8×10 6 kg / m 4 , about 9×10 6 kg / m 4 , about 1×10 7 kg / m 4 , about 2×10 7 kg / m 4 , about 3×10 7 kg / m 4 , about 4×10 7 kg / m 4 , about 5×10 7 kg / m 4 , about 6×10 7 kg / m 4 , about 7×10 7 kg / m 4 , about 8×107 kg / m 4 、 about 9×10 7 kg / m 4 、 about 1×10 8 kg / m 4 、 about 2×10 8 kg / m 4 、 about 3×10 8 kg / m 4 、 about 4×10 8 kg / m 4 、 about 5×10 8 kg / m 4 、 about 6×10 8 kg / m 4 、 about 7×10 8 kg / m 4 、 about 8×10 8 kg / m 4 、 about 9×10 8 kg / m 4 、 or about 1×10 9 kg / m 4 and can have an average concentration gradient of.

[0048] In some embodiments, the cathode 210 can have a viscosity (at 25 °C) of at least about 100 Pa·s, at least about 150 Pa·s, at least about 200 Pa·s, at least about 250 Pa·s, at least about 300 Pa·s, at least about 350 Pa·s, at least about 400 Pa·s, at least about 450 Pa·s, at least about 500 Pa·s, at least about 550 Pa·s, at least about 600 Pa·s, at least about 650 Pa·s, at least about 700 Pa·s, at least about 750 Pa·s, at least about 800 Pa·s, at least about 850 Pa·s, at least about 900 Pa·s, or at least about 950 Pa·s. In some embodiments, the cathode 210 can have a viscosity of about 1,000 Pa·s or less, about 950 Pa·s or less, about 900 Pa·s or less, about 850 Pa·s or less, about 800 Pa·s or less, about 750 Pa·s or less, about 700 Pa·s or less, about 650 Pa·s or less, about 600 Pa·s or less, about 550 Pa·s or less, about 500 Pa·s or less, about 450 Pa·s or less, about 400 Pa·s or less, about 350 Pa·s or less, about 300 Pa·s or less, about 250 Pa·s or less, about 200 Pa·s or less, or about 950 Pa·s or less. Combinations of the viscosities above are also possible (e.g., at least about 100 Pa·s or more and about 1,000 Pa·s or less, or at least about 300 Pa·s or more and about 600 Pa·s or less), including all values and ranges therebetween. In some embodiments, the cathode 210 can have a viscosity of about 100 Pa·s, about 150 Pa·s, about 200 Pa·s, about 250 Pa·s, about 300 Pa·s, about 350 Pa·s, about 400 Pa·s, about 450 Pa·s, about 500 Pa·s, about 550 Pa·s, about 600 Pa·s, about 650 Pa·s, about 700 Pa·s, about 750 Pa·s, about 800 Pa·s, about 850 Pa·s, about 900 Pa·s, about 950 Pa·s, or about 1,000 Pa·s.

[0049] In some embodiments, the cathode 210 can have a viscosity gradient. In some embodiments, the viscosity gradient can exist while the electrochemical cell 200 is charging. In some embodiments, the viscosity gradient can exist while the electrochemical cell 200 is discharging. In some embodiments, the viscosity gradient can exist while the electrochemical cell 200 is resting. In some embodiments, the cathode 210 is at least about 1×10 5 Pa·s / m, at least about 2×10 5 Pa·s / m, at least about 3×10 5 Pa·s / m, at least about 4×10 5 Pa·s / m, at least about 5×10 5 Pa·s / m, at least about 6×10 5 Pa·s / m, at least about 7×10 5 Pa·s / m, at least about 8×10 5 Pa·s / m, at least about 9×10 5 Pa·s / m, at least about 1×10 6 Pa·s / m, at least about 2×10 6 Pa·s / m, at least about 3×10 6 Pa·s / m, at least about 4×10 6 Pa·s / m, at least about 5×10 6 Pa·s / m, at least about 6×10 6 Pa·s / m, at least about 7×10 6 Pa·s / m, at least about 8×10 6 Pa·s / m, at least about 9×10 6 Pa·s / m, at least about 1×10 7 Pa·s / m, at least about 2×10 7 Pa·s / m, at least about 3×10 7 Pa·s / m, at least about 4×10 7 Pa·s / m, at least about 5×10 7 Pa·s / m, at least about 6×10 7 Pa·s / m, at least about 7×10 7 Pa·s / m, at least about 8×10 7 Pa·s / m, at least about 9×10 7Pa·s / m, at least about 1×10 8 Pa·s / m, at least about 2×10 8 Pa·s / m, at least about 3×10 8 Pa·s / m, at least about 4×10 8 Pa·s / m, at least about 5×10 8 Pa·s / m, at least about 6×10 8 Pa·s / m, at least about 7×10 8 Pa·s / m, at least about 8×10 8 Pa·s / m, or at least about 9×10 8 Pa·s / m can have an average viscosity gradient. In some embodiments, the cathode 210 is about 1×10 9 Pa·s / m or less, about 9×10 8 Pa·s / m or less, about 8×10 8 Pa·s / m or less, about 7×10 8 Pa·s / m or less, about 6×10 8 Pa·s / m or less, about 5×10 8 Pa·s / m or less, about 4×10 8 Pa·s / m or less, about 3×10 8 Pa·s / m or less, about 2×10 8 Pa·s / m or less, about 1×10 8 Pa·s / m or less, about 9×10 7 Pa·s / m or less, about 8×10 7 Pa·s / m or less, about 7×10 7 Pa·s / m or less, about 6×10 7 Pa·s / m or less, about 5×10 7 Pa·s / m or less, about 4×10 7 Pa·s / m or less, about 3×10 7 Pa·s / m or less, about 2×10 7 Pa·s / m or less, about 1×10 7 Pa·s / m or less, about 9×10 6 Pa·s / m or less, about 8×10 6 Pa·s / m or less, about 7×10 6 Pa·s / m or less, about 6×10 6 Pa·s / m or less, about 5×10 6 Pa·s / m or less, about 4×10 6 Pa·s / m or less, about 3×106 Less than Pa·s / m, about 2×10 6 Less than Pa·s / m, about 1×10 6 Less than Pa·s / m, about 9×10 5 Less than Pa·s / m, about 8×10 5 Less than Pa·s / m, about 7×10 5 Less than Pa·s / m, about 6×10 5 Less than Pa·s / m, about 5×10 5 Less than Pa·s / m, about 4×10 5 Less than Pa·s / m, about 3×10 5 Less than Pa·s / m, or about 2×10 5 It can have an average viscosity gradient of less than Pa·s / m.

[0050] The above combinations of average viscosity gradients are also possible (for example, at least about 1×10 5 Pa·s / m and about 1×10 9 Pa·s / m or less, or at least about 1×10 6 Pa·s / m and about 1×10 8 Pa·s / m or less), including all values and ranges therebetween. In some embodiments, the cathode 210 is about 1×10 5 Pa·s / m, about 2×10 5 Pa·s / m, about 3×10 5 Pa·s / m, about 4×10 5 Pa·s / m, about 5×105Pa·s / m, about 6×10 5 Pa·s / m, about 7×10 5 Pa·s / m, about 8×10 5 Pa·s / m, about 9×10 5 Pa·s / m, about 1×10 6 Pa·s / m, about 2×10 6 Pa·s / m, about 3×10 6 Pa·s / m, about 4×10 6 Pa·s / m, about 5×10 6 Pa·s / m, about 6×10 6 Pa·s / m, about 7×10 6 Pa·s / m, about 8×10 6 Pa·s / m, about 9×10 6 Pa·s / m, about 1×10 7 Pa·s / m, about 2×107 Pa·s / m, about 3×10 7 Pa·s / m, about 4×10 7 Pa·s / m, about 5×10 7 Pa·s / m, about 6×10 7 Pa·s / m, about 7×10 7 Pa·s / m, about 8×10 7 Pa·s / m, about 9×10 7 Pa·s / m, about 1×10 8 Pa·s / m, about 2×10 8 Pa·s / m, about 3×10 8 Pa·s / m, about 4×10 8 Pa·s / m, about 5×10 8 Pa·s / m, about 6×10 8 Pa·s / m, about 7×10 8 Pa·s / m, about 8×10 8 Pa·s / m, about 9×10 8 Pa·s / m, or about 1×10 9 Pa·s / m can have an average viscosity gradient of

[0051] In some embodiments, the cathode current collector 220 can be composed of copper, aluminum, titanium, or any combination thereof. In some embodiments, the cathode current collector 220 can have a thickness of at least about 1 μm, at least about 2 μm, at least about 3 μm, at least about 4 μm, at least about 5 μm, at least about 10 μm, at least about 15 μm, at least about 20 μm, at least about 25 μm, at least about 30 μm, at least about 35 μm, at least about 40 μm, or at least about 45 μm. In some embodiments, the cathode current collector 220 can have a thickness of about 50 μm or less, about 45 μm or less, about 40 μm or less, about 35 μm or less, about 30 μm or less, about 25 μm or less, about 20 μm or less, about 15 μm or less, about 10 μm or less, about 5 μm or less, about 4 μm or less, about 3 μm or less, or about 2 μm or less. Combinations of the above thicknesses of the cathode current collector 220 are also possible (e.g., at least about 1 μm or more and about 50 μm or less, or at least about 5 μm or more and about 20 μm or less), including all values and ranges therebetween. In some embodiments, the cathode current collector 220 can have a thickness of about 1 μm, about 2 μm, about 3 μm, about 4 μm, about 5 μm, about 10 μm, about 15 μm, about 20 μm, about 25 μm, about 30 μm, about 35 μm, about 40 μm, about 45 μm, or about 50 μm.

[0052] In some embodiments, the anode 230 can include a semi-solid anode. In some embodiments, the anode 230 can have a thickness of at least about 100 μm, at least about 150 μm, at least about 200 μm, at least about 250 μm, at least about 300 μm, at least about 350 μm, at least about 400 μm, at least about 450 μm, at least about 500 μm, at least about 550 μm, at least about 600 μm, at least about 650 μm, at least about 700 μm, at least about 750 μm, at least about 800 μm, at least about 850 μm, at least about 900 μm, at least about 950 μm, at least about 1,000 μm, at least about 1,050 μm, at least about 1,100 μm, at least about 1,150 μm, at least about 1,200 μm, at least about 1,250 μm, at least about 1,300 μm, at least about 1,350 μm, at least about 1,400 μm, at least about 1,450 μm, at least about 1,500 μm, at least about 1,550 μm, at least about 1,600 μm, at least about 1,650 μm, at least about 1,700 μm, at least about 1,750 μm, at least about 1,800 μm, at least about 1,850 μm, at least about 1,900 μm, or at least about 1,950 μm. In some embodiments, the anode 230 can have a thickness of about 2,000 μm or less, about 1,950 μm or less, about 1,900 μm or less, about 1,850 μm or less, about 1,800 μm or less, about 1,750 μm or less, about 1,700 μm or less, about 1,650 μm or less, about 1,600 μm or less, about 1,550 μm or less, about 1,500 μm or less, about 1,450 μm or less, about 1,400 μm or less, about 1,350 μm or less, about 1,300 μm or less, about 1,250 μm or less, about 1,200 μm or less, about 1,150 μm or less, about 1,100 μm or less, about 1,050 μm or less, about 1,000 μm or less, about 950 μm or less, about 900 μm or less, about 850 μm or less, about 800 μm or less, about 750 μm or less, about 700 μm or less, about 650 μm or less, about 600 μm or less, about 550 μm or less, about 500 μm or less, about 450 μm or less, about 400 μm or less, about 350 μm or less, about 300 μm or less, about 250 μm or less, about 200 μm or less, or about 150 μm or less.The above thickness combinations are also possible (e.g., at least about 100 μm and about 2,000 μm or less, or at least about 300 μm and about 1,000 μm or less), including all values and ranges therebetween. In some embodiments, the anode 230 can have a thickness of about 100 μm, about 150 μm, about 200 μm, about 250 μm, about 300 μm, about 350 μm, about 400 μm, about 450 μm, about 500 μm, about 550 μm, about 600 μm, about 650 μm, about 700 μm, about 750 μm, about 800 μm, about 850 μm, about 900 μm, about 950 μm, about 1,000 μm, about 1,050 μm, about 1,100 μm, about 1,150 μm, about 1,200 μm, about 1,250 μm, about 1,300 μm, about 1,350 μm, about 1,400 μm, about 1,450 μm, about 1,500 μm, about 1,550 μm, about 1,600 μm, about 1,650 μm, about 1,700 μm, about 1,750 μm, about 1,800 μm, about 1,850 μm, about 1,900 μm, about 1,950 μm, or about 2,000 μm.

[0053] In some embodiments, the anode 230 is at least about 1,000 mol / m 3 at least about 1,500 mol / m 3 at least about 2,000 mol / m 3 at least about 2,500 mol / m 3 at least about 3,000 mol / m 3 at least about 3,500 mol / m 3 at least about 4,000 mol / m 3 at least about 4,500 mol / m 3 at least about 5,000 mol / m 3 at least about 5,500 mol / m 3 at least about 6,000 mol / m 3 at least about 6,500 mol / m 3 at least about 7,000 mol / m 3 at least about 7,500 mol / m 3 at least about 8,000 mol / m 3 at least about 8,500 mol / m 3 at least about 9,000 mol / m3 or has an electrolyte salt concentration of at least about 9,500 mol / m 3 . In some embodiments, the anode 230 has an electrolyte salt concentration of about 10,000 mol / m 3 or less, about 9,500 mol / m 3 or less, about 9,000 mol / m 3 or less, about 8,500 mol / m 3 or less, about 8,000 mol / m 3 or less, about 7,500 mol / m 3 or less, about 7,000 mol / m 3 or less, about 6,500 mol / m 3 or less, about 6,000 mol / m 3 or less, about 5,500 mol / m 3 or less, about 5,000 mol / m 3 or less, about 4,500 mol / m 3 or less, about 4,000 mol / m 3 or less, about 3,500 mol / m 3 or less, about 3,000 mol / m 3 or less, or about 2,500 mol / m 3 or less, about 2,000 mol / m 3 or less, or about 1,500 mol / m 3 or less. Combinations of the above electrolyte salt concentrations in the anode 230 are also possible (e.g., at least about 1,000 mol / m 3 at about 10,000 mol / m 3 or less, or at least about 2,000 mol / m 3 at about 5,000 mol / m 3 or less), including all values and ranges therebetween. In some embodiments, the anode 230 has an electrolyte salt concentration of about 1,000 mol / m 3 , about 1,500 mol / m 3 , about 2,000 mol / m 3 , about 2,500 mol / m 3 , about 3,000 mol / m 3 , about 3,500 mol / m 3 , about 4,000 mol / m 3 , about 4,500 mol / m 3 , about 5,000 mol / m 3, about 5,500 mol / m 3 , about 6,000 mol / m 3 , about 6,500 mol / m 3 , about 7,000 mol / m 3 , about 7,500 mol / m 3 , about 8,000 mol / m 3 , about 8,500 mol / m 3 , about 9,000 mol / m 3 , about 9,500 mol / m 3 , or about 10,000 mol / m 3 and can have an electrolyte salt concentration of.

[0054] In some embodiments, the anode 230 can have an electrolyte salt concentration gradient along the thickness of the anode 230. In some embodiments, the concentration gradient can exist while the electrochemical cell 200 is charging. In some embodiments, the concentration gradient can exist while the electrochemical cell 200 is discharging. In some embodiments, the concentration gradient can exist while the electrochemical cell 200 is in a resting state. In some embodiments, the anode 230 is at least about 1.0×10 7 mol / m 4 , at least about 1.1×10 7 mol / m 4 , at least about 1.2×10 7 mol / m 4 , at least about 1.3×10 7 mol / m 4 , at least about 1.4×10 7 mol / m 4 , at least about 1.5×10 7 mol / m 4 , at least about 1.6×10 7 mol / m 4 , at least about 1.7×10 7 mol / m 4 , at least about 1.8×10 7 mol / m 4 , at least about 1.9×10 7 mol / m 4 , at least about 2.0×10 7 mol / m 4, at least about 2.1×10 7 mol / m 4 , at least about 2.2×10 7 mol / m 4 , at least about 2.3×10 7 mol / m 4 , at least about 2. 4 ×10 7 mol / m 4 , at least about 2.5×10 7 mol / m 4 , at least about 2.6×10 7 mol / m 4 , at least about 2.7×10 7 mol / m 4 , at least about 2.8×10 7 mol / m 4 , at least about 2.9×10 7 mol / m 4 , at least about 3.0×10 7 mol / m 4 , at least about 3.1×10 7 mol / m 4 , at least about 3.2×10 7 mol / m 4 , at least about 3.3×10 7 mol / m 4 , at least about 3.4×10 7 mol / m 4 , at least about 3.5×10 7 mol / m 4 , at least about 3.6×10 7 mol / m 4 , at least about 3.7×10 7 mol / m 4 , at least about 3.8×10 7 mol / m 4 , at least about 3.9×10 7 mol / m 4 , at least about 4.0×10 7 mol / m 4 , at least about 4.1×10 7 mol / m 4 , at least about 4.2×10 7 mol / m 4 , at least about 4.3×107 mol / m 4 and at least about 4.4×10 7 mol / m 4 and at least about 4.5×10 7 mol / m4 and at least about 4.6×10 7 mol / m 4 and at least about 4.7×10 7 mol / m 4 and at least about 4.8×107mol / m 4 and at least about 4.9×10 7 mol / m 4 can have an average electrolyte salt concentration gradient. In some embodiments, anode 230 is about 5.0×10 7 mol / m 4 or less, about 4.9×10 7 mol / m 4 or less, about 4.8×10 7 mol / m 4 or less, about 4.7×10 7 mol / m 4 or less, about 4.6×10 7 mol / m 4 or less, about 4.5×10 7 mol / m 4 or less, about 4.4×10 7 mol / m 4 or less, about 4.3x10 7 mol / m 4 or less, about 4.2x10 7 mol / m 4 or less, about 4.1x10 7 mol / m 4 or less, about 4.0x10 7 mol / m 4 or less, about 3.9x10 7 mol / m 4 or less, about 3.8×10 7 mol / m 4 or less, about 3.7×10 7 mol / m 4 or less, about 3.6×10 7 mol / m 4 or less, about 3.5×10 7 mol / m 4 or less, about 3.4×10 7 mol / m4 The following is about 3.3×10 7 mol / m 4 The following is about 3.2x10 7 mol / m 4 The following is about 3.1x10 7 mol / m 4 The following is about 3.0x10 7 mol / m 4 The following is about 2.9x10 7 mol / m 4 The following is about 2.8x10 7 mol / m 4 The following is about 2.7x10 7 mol / m 4 The following is about 2.6x10 7 mol / m 4 The following is about 2.5x10 7 mol / m 4 The following is about 2.4x10 7 mol / m 4 The following is about 2.3x10 7 mol / m 4 The following is about 2.2x10 7 mol / m 4 The following is about 2.1×10 7 mol / m 4 The following is about 2.0×10 7 mol / m 4 The following is about 1.9×10 7 mol / m 4 The following is about 1.8×10 7 mol / m 4 The following is about 1.7×10 7 mol / m 4 The following is about 1.6×10 7 mol / m 4 The following is about 1.5×10 7 mol / m 4 The following is about 1.4×10 7 mol / m 4 The following is about 1.3×10 7 mol / m 4 The following is about 1.2×10 7 mol / m 4 The following is, or about 1.1×10 7 mol / m 4 It can have an average electrolyte salt concentration gradient below the following.

[0055] The above combinations of average electrolyte salt concentrations are also possible (for example, at least about 1×10 7 mol / m 4 or more and about 5 mol / m 4 or less, or at least about 2 mol / m 4 or more and about 4 mol / m 4 or less), including all values and ranges therebetween. In some embodiments, the anode 230 is about 1.0×10 7 mol / m 4 , about 1.1×10 7 mol / m 4 , about 1.2×10 7 mol / m 4 , about 1.3×10 7 mol / m 4 , about 1.4×10 7 mol / m 4 , about 1.5×10 7 mol / m 4 , about 1.6×10 7 mol / m 4 , about 1.7×10 7 mol / m 4 , about 1.8×10 7 mol / m 4 , about 1.9×10 7 mol / m 4 , about 2.0×10 7 mol / m 4 , about 2.1×10 7 mol / m 4 , about 2.2×10 7 mol / m 4 , about 2.3×10 7 mol / m4, about 2.4×10 7 mol / m 4 , about 2.5×10 7 mol / m 4 , about 2.6×10 7 mol / m 4 , about 2.7×10 7 mol / m 4 , about 2.8×10 7 mol / m 4 , about 2.9×10 7 mol / m 4 , about 3.0×10 7mol / m 4 、 about 3.1×10 7 mol / m 4 、 about 3.2×10 7 mol / m 4 、 about 3.3×10 7 mol / m 4 、 about 3.4×10 7 mol / m 4 、 about 3.5×10 7 mol / m 4 、 about 3.6×10 7 mol / m 4 、 about 3.7×10 7 mol / m 4 、 about 3.8×10 7 mol / m 4 、 about 3.9×10 7 mol / m 4 、 about 4.0×10 7 mol / m 4 、 about 4.1×10 7 mol / m 4 、 about 4.2×10 7 mol / m 4 、 about 4.3×10 7 mol / m 4 、 about 4.4×10 7 mol / m 4 、 about 4.5×10 7 mol / m 4 、 about 4.6×10 7 mol / m 4 、 about 4.7×10 7 mol / m 4 、 about 4.8×10 7 mol / m 4 、 about 4.9×10 7 mol / m 4 、 or about 5.0×10 7 mol / m 4 and can have an average electrolyte salt concentration gradient.

[0056] In some embodiments, the anode 230 can have a density gradient. In some embodiments, the density gradient can exist while the electrochemical cell 200 is charging. In some embodiments, the density gradient can exist while the electrochemical cell 200 is discharging. In some embodiments, the density gradient can exist while the electrochemical cell 200 is at rest. In some embodiments, the anode 230 is at least about 1×10 5 kg / m 4 、 at least about 2×10 5 kg / m 4 、 at least about 3×10 5 kg / m 4 、 at least about 4×10 5 kg / m 4 、 at least about 5×10 5 kg / m 4 、 at least about 6×10 5 kg / m 4 、 at least about 7×10 5 kg / m 4 、 at least about 8×10 5 kg / m 4 、 at least about 9×10 5 kg / m 4 、 at least about 1×106 kg / m 4 、 at least about 2×10 6 kg / m 4 、 at least about 3×10 6 kg / m 4 、 at least about 4×106 kg / m 4 、 at least about 5×10 6 kg / m 4 、 at least about 6×10 6 kg / m 4 、 at least about 7×106 kg / m 4 、 at least about 8×10 6 kg / m 4 、 at least about 9×10 6 kg / m 4 、 at least about 1×107 kg / m 4 、 at least about 2×10 7 kg / m 4 、 at least about 3×10 7 kg / m4 and having an average density gradient of at least about 4×107 kg / m 4 and having an average density gradient of at least about 5×10 7 kg / m 4 and having an average density gradient of at least about 6×10 7 kg / m 4 and having an average density gradient of at least about 7×107 kg / m 4 and having an average density gradient of at least about 8×10 7 kg / m 4 and having an average density gradient of at least about 9×10 7 kg / m 4 and having an average density gradient of at least about 1×108 kg / m 4 and having an average density gradient of at least about 2×10 8 kg / m 4 and having an average density gradient of at least about 3×10 8 kg / m 4 and having an average density gradient of at least about 4×108 kg / m 4 and having an average density gradient of at least about 5×10 8 kg / m 4 and having an average density gradient of at least about 6×10 8 kg / m 4 and having an average density gradient of at least about 7×108 kg / m 4 and having an average density gradient of at least about 8×10 8 kg / m 4 or having an average density gradient of at least about 9×10 8 kg / m 4 can have. In some embodiments, the anode 230 is about 1×10 9 kg / m 4 or less, about 9×10 8 kg / m 4 or less, about 8×10 8 kg / m 4 or less, about 7×10 8 kg / m 4 or less, about 6×10 8 kg / m 4 or less, about 5×10 8 kg / m 4 or less, about 4×10 8 kg / m 4 or less, about 3×10 8 kg / m 4 or less, about 2×10 8 kg / m 4 or less, about 1×10 8 kg / m 4 or less, about 9×10 7kg / m 4 Hereinafter, about 8×10 7 kg / m 4 Hereinafter, about 7×10 7 kg / m 4 Hereinafter, about 6×10 7 kg / m 4 Hereinafter, about 5×10 7 kg / m 4 Hereinafter, about 4×10 7 kg / m 4 Hereinafter, about 3×10 7 kg / m 4 Hereinafter, about 2×10 7 kg / m 4 Hereinafter, about 1×10 7 kg / m 4 Hereinafter, about 9×10 6 kg / m 4 Hereinafter, about 8×10 6 kg / m 4 Hereinafter, about 7×10 6 kg / m 4 Hereinafter, about 6×10 6 kg / m 4 Hereinafter, about 5×10 6 kg / m 4 Hereinafter, about 4×10 6 kg / m 4 Hereinafter, about 3×10 6 kg / m 4 Hereinafter, about 2×10 6 kg / m 4 Hereinafter, about 1×10 6 kg / m 4 Hereinafter, about 9×10 5 kg / m 4 Hereinafter, about 8×10 5 kg / m 4 Hereinafter, about 7×10 5 kg / m 4 Hereinafter, about 6×10 5 kg / m 4 Hereinafter, about 5×10 5 kg / m 4 Hereinafter, about 4×10 5 kg / m 4 Hereinafter, about 3×10 5 kg / m 4 Hereinafter, or about 2×10 5 kg / m 4 It can have an average density gradient of hereinafter.

[0057] The above combinations of average density gradients are also possible (e.g., at least about 1×10 5 kg / m 4 or more and about 1×10 9 kg / m 4 or less, or at least about 1×10 6 kg / m 4 or more and about 1×10 8 kg / m 4 or less), including all values and ranges therebetween. In some embodiments, anode 230 is about 1×10 5 kg / m 4 , about 2×10 5 kg / m 4 , about 3×10 5 kg / m 4 , about 4×10 5 kg / m4, about 5×10 5 kg / m 4 , about 6×10 5 kg / m 4 , about 7×10 5 kg / m 4 , about 8×10 5 kg / m 4 , about 9×10 5 kg / m 4 , about 1×10 6 kg / m 4 , about 2×10 6 kg / m 4 , about 3×10 6 kg / m 4 , about 4×10 6 kg / m 4 , about 5×10 6 kg / m 4 , about 6×10 6 kg / m 4 , about 7×10 6 kg / m4, about 8×10 6 kg / m 4 , about 9×10 6 kg / m 4 , about 1×10 7 kg / m 4 , about 2×10 7 kg / m 4 , about 3×10 7 kg / m 4 , about 4×10 7kg / m 4 、 about 5×10 7 kg / m 4 、 about 6×10 7 kg / m 4 、 about 7×10 7 kg / m 4 、 about 8×10 7 kg / m 4 、 about 9×10 7 kg / m 4 、 about 1×10 8 kg / m 4 、 about 2×10 8 kg / m 4 、 about 3×10 8 kg / m 4 、 about 4×10 8 kg / m 4 、 about 5×10 8 kg / m 4 、 about 6×10 8 kg / m 4 、 about 7×10 8 kg / m 4 、 about 8×10 8 kg / m 4 、 about 9×10 8 kg / m 4 、 or about 1×10 9 kg / m 4 and can have an average density gradient of.

[0058] In some embodiments, the anode 230 can have a viscosity (at 25 °C) of at least about 100 Pa·s, at least about 150 Pa·s, at least about 200 Pa·s, at least about 250 Pa·s, at least about 300 Pa·s, at least about 350 Pa·s, at least about 400 Pa·s, at least about 450 Pa·s, at least about 500 Pa·s, at least about 550 Pa·s, at least about 600 Pa·s, at least about 650 Pa·s, at least about 700 Pa·s, at least about 750 Pa·s, at least about 800 Pa·s, at least about 850 Pa·s, at least about 900 Pa·s, or at least about 950 Pa·s. In some embodiments, the anode 230 can have a viscosity of about 1,000 Pa·s or less, about 950 Pa·s or less, about 900 Pa·s or less, about 850 Pa·s or less, about 800 Pa·s or less, about 750 Pa·s or less, about 700 Pa·s or less, about 650 Pa·s or less, about 600 Pa·s or less, about 550 Pa·s or less, about 500 Pa·s or less, about 450 Pa·s or less, about 400 Pa·s or less, about 350 Pa·s or less, about 300 Pa·s or less, about 250 Pa·s or less, about 200 Pa·s or less, or about 150 Pa·s or less. Combinations of the viscosities described above are also possible (e.g., at least about 100 Pa·s or more and about 1,000 Pa·s or less, or at least about 300 Pa·s or more and about 600 Pa·s or less), including all values and ranges therebetween. In some embodiments, the anode 230 can have a viscosity of about 100 Pa·s, about 150 Pa·s, about 200 Pa·s, about 250 Pa·s, about 300 Pa·s, about 350 Pa·s, about 400 Pa·s, about 450 Pa·s, about 500 Pa·s, about 550 Pa·s, about 600 Pa·s, about 650 Pa·s, about 700 Pa·s, about 750 Pa·s, about 800 Pa·s, about 850 Pa·s, about 900 Pa·s, about 950 Pa·s, or about 1,000 Pa·s.

[0059] In some embodiments, the anode 230 can have a viscosity gradient. In some embodiments, the viscosity gradient can be present while the electrochemical cell 200 is charging. In some embodiments, the viscosity gradient can be present while the electrochemical cell 200 is discharging. In some embodiments, the viscosity gradient can be present while the electrochemical cell 200 is resting. In some embodiments, the anode 210 is at least about 1×10 5 Pa·s / m, at least about 2×10 5 Pa·s / m, at least about 3×10 5 Pa·s / m, at least about 4×10 5 Pa·s / m, at least about 5×10 5 Pa·s / m, at least about 6×10 5 Pa·s / m, at least about 7×10 5 Pa·s / m, at least about 8×10 5 Pa·s / m, at least about 9×10 5 Pa·s / m, at least about 1×10 6 Pa·s / m, at least about 2×10 6 Pa·s / m, at least about 3×10 6 Pa·s / m, at least about 4×10 6 Pa·s / m, at least about 5×10 6 Pa·s / m, at least about 6×10 6 Pa·s / m, at least about 7×10 6 Pa·s / m, at least about 8×10 6 Pa·s / m, at least about 9×10 6 Pa·s / m, at least about 1×10 7 Pa·s / m, at least about 2×10 7 Pa·s / m, at least about 3×10 7 Pa·s / m, at least about 4×10 7 Pa·s / m, 5×10 7 Pa·s / m, at least about 6×10 7 Pa·s / m, at least about 7×10 7 Pa·s / m, at least about 8×10 7 Pa·s / m, at least about 9×10 7 Pa·s / m, at least about 1×108 Pa·s / m, at least about 2×10 8 Pa·s / m, at least about 3×10 8 Pa·s / m, at least about 4×10 8 Pa·s / m, at least about 5×10 8 Pa·s / m, at least about 6×10 8 Pa·s / m, at least about 7×10 8 Pa·s / m, at least about 8×10 8 Pa·s / m, or at least about 9×10 8 Pa·s / m and can have an average viscosity gradient. In some embodiments, the anode 210 is about 1×10 9 Pa·s / m or less, about 9×10 8 Pa·s / m or less, about 8×10 8 Pa·s / m or less, about 7×10 8 Pa·s / m or less, about 6×10 8 Pa·s / m or less, about 5×10 8 Pa·s / m or less, about 4×10 8 Pa·s / m or less, about 3×10 8 Pa·s / m or less, about 2×10 8 Pa·s / m or less, about 1×10 8 Pa·s / m or less, about 9×10 7 Pa·s / m or less, about 8×10 7 Pa·s / m or less, about 7×10 7 Pa·s / m or less, about 6×10 7 Pa·s / m or less, about 5×10 7 Pa·s / m or less, about 4×10 7 Pa·s / m or less, about 3×10 7 Pa·s / m or less, about 2×10 7 Pa·s / m or less, about 1×10 7 Pa·s / m or less, about 9×10 6 Pa·s / m or less, about 8×10 6 Pa·s / m or less, about 7×10 6 Pa·s / m or less, about 6×10 6 Pa·s / m or less, about 5×10 6 Pa·s / m or less, about 4×10 6 Pa·s / m or less, about 3×10 6Less than Pa·s / m, about 2×10 6 Less than Pa·s / m, about 1×10 6 Less than Pa·s / m, about 9×10 5 Less than Pa·s / m, about 8×10 5 Less than Pa·s / m, about 7×10 5 Less than Pa·s / m, about 6×10 5 Less than Pa·s / m, about 5×10 5 Less than Pa·s / m, about 4×10 5 Less than Pa·s / m, about 3×10 5 Less than Pa·s / m, or about 2×10 5 Less than Pa·s / m can have an average viscosity gradient.

[0060] The above combinations of average viscosity gradients are also possible (for example, at least about 1×10 5 Pa·s / m and about 1×10 9 Pa·s / m or less, or at least about 1×10 6 Pa·s / m and about 1×10 8 Pa·s / m or less), including all values and ranges therebetween. In some embodiments, the anode 230 is about 1×10 5 Pa·s / m, about 2×10 5 Pa·s / m, about 3×10 5 Pa·s / m, about 4×10 5 Pa·s / m, about 5×10 5 Pa·s / m, about 6×10 5 Pa·s / m, about 7×10 5 Pa·s / m, about 8×10 5 Pa·s / m, about 9×10 5 Pa·s / m, about 1×10 6 Pa·s / m, about 2×10 6 Pa·s / m, about 3×10 6 Pa·s / m, about 4×10 6 Pa·s / m, about 5×10 6 Pa·s / m, about 6×10 6 Pa·s / m, about 7×10 6 Pa·s / m, about 8×10 6 Pa·s / m, about 9×10 6 Pa·s / m, about 1×10 7 Pa·s / m, about 2×107 Pa·s / m, about 3×10 7 Pa·s / m, about 4×10 7 Pa·s / m, about 5×10 7 Pa·s / m, about 6×10 7 Pa·s / m, about 7×10 7 Pa·s / m, about 8×10 7 Pa·s / m, about 9×10 7 Pa·s / m, about 1×10 8 Pa·s / m, about 2×10 8 Pa·s / m, about 3×10 8 Pa·s / m, about 4×10 8 Pa·s / m, about 5×10 8 Pa·s / m, about 6×10 8 Pa·s / m, about 7×10 8 Pa·s / m, about 8×10 8 Pa·s / m, about 9×10 8 Pa·s / m, or about 1×10 9 Pa·s / m can have an average viscosity gradient of.

[0061] In some embodiments, the anode current collector 240 can comprise aluminum or any other suitable current collector material. In some embodiments, the anode current collector 240 can have a thickness of at least about 1 μm, at least about 2 μm, at least about 3 μm, at least about 4 μm, at least about 5 μm, at least about 10 μm, at least about 15 μm, at least about 20 μm, at least about 25 μm, at least about 30 μm, at least about 35 μm, at least about 40 μm, or at least about 45 μm. In some embodiments, the anode current collector 240 can have a thickness of about 50 μm or less, about 45 μm or less, about 40 μm or less, about 35 μm or less, about 30 μm or less, about 25 μm or less, about 20 μm or less, about 15 μm or less, about 10 μm or less, about 5 μm or less, about 4 μm or less, about 3 μm or less, or about 2 μm or less. Combinations of the above thicknesses of the anode current collector 240 are also possible (e.g., at least about 1 μm to about 50 μm or at least about 5 μm to about 20 μm), including all values and ranges therebetween. In some embodiments, the anode current collector 240 can have a thickness of about 1 μm, about 2 μm, about 3 μm, about 4 μm, about 5 μm, about 10 μm, about 15 μm, about 20 μm, about 25 μm, about 30 μm, about 35 μm, about 40 μm, about 45 μm, or about 50 μm.

[0062] Separator 250 can include any suitable separator that functions as an ion-permeable membrane. In other words, separator 250 enables ion exchange while maintaining physical separation between anode 230 and cathode 210. For example, separator 250 can be any conventional membrane capable of ion transport. In some embodiments, separator 250 is a liquid-impermeable membrane that permits ion transport therethrough, i.e., a solid or gel ion conductor. In some embodiments, separator 250 is a porous polymer membrane infused with a liquid electrolyte that allows ion shuttling between the electroactive materials of anode 230 and cathode 210 while preventing electron movement. In some embodiments, separator 250 can be a microporous membrane that prevents particles forming the positive and negative compositions from crossing the membrane. For example, the membrane material can be selected from polyethylene oxide (PEO) polymers complexed with lithium salts to have lithium conductivity, and Nafion™ membranes which are proton conductors. For example, a PEO-based electrolyte can be used as the membrane, which is pinhole-free, a solid ion conductor, and optionally can be stabilized with other membranes such as glass fiber separators as a support layer. PEO can also be used as a slurry stabilizer, dispersant, etc. for positive or negative redox compositions. PEO is stable even when in contact with typical alkyl carbonate-based electrolytes. This is particularly useful in phosphate-based cell chemistries where the anode cell potential is less than about 3.6V versus Li metal. The operating temperature of the redox cell can be increased as needed to improve the ion conductivity of the membrane. In some embodiments, separator 250 can include polyethylene, polypropylene, polyimide, or any combination thereof.

[0063] In some embodiments, separator 250 can have a thickness of at least about 5 μm, at least about 10 μm, at least about 15 μm, at least about 20 μm, at least about 25 μm, at least about 30 μm, at least about 35 μm, at least about 40 μm, or at least about 45 μm. In some embodiments, separator 250 can have a thickness of about 50 μm or less, about 45 μm or less, about 40 μm or less, about 35 μm or less, about 30 μm or less, about 25 μm or less, about 20 μm or less, about 15 μm or less, or about 10 μm or less. Combinations of the above thicknesses are also possible (e.g., at least about 5 μm to about 50 μm or at least about 10 μm to about 30 μm), including all values and ranges therebetween. In some embodiments, separator 250 can have a thickness of about 5 μm, about 10 μm, about 15 μm, about 20 μm, about 25 μm, about 30 μm, about 35 μm, about 40 μm, about 45 μm, or about 50 μm.

[0064] In some embodiments, carbon coating 260 can include any of the substances listed above with respect to the carbon coating applied in step 15. In some embodiments, carbon coating 260 can be mixed with an electrolyte solution. In some embodiments, carbon coating 260 can be mixed with the same electrolyte solution as cathode 230. In some embodiments, carbon coating 260 can have a thickness of at least about 500 nm, at least about 1 μm, at least about 2 μm, at least about 3 μm, at least about 4 μm, at least about 5 μm, at least about 6 μm, at least about 7 μm, at least about 8 μm, at least about 9 μm, at least about 10 μm, at least about 11 μm, at least about 12 μm, at least about 13 μm, at least about 14 μm, at least about 15 μm, at least about 16 μm, at least about 17 μm, at least about 18 μm, or at least about 19 μm. In some embodiments, carbon coating 260 can have a thickness of about 20 μm or less, about 19 μm or less, about 18 μm or less, about 17 μm or less, about 16 μm or less, about 15 μm or less, about 14 μm or less, about 13 μm or less, about 12 μm or less, about 11 μm or less, about 10 μm or less, about 9 μm or less, about 8 μm or less, about 7 μm or less, about 6 μm or less, about 5 μm or less, about 4 μm or less, about 3 μm or less, about 2 μm or less, or about 1 μm or less. The above combinations of thicknesses of carbon coating 260 are also possible (e.g., at least about 500 nm or more and about 20 μm or less, or at least about 5 μm or more and about 15 μm or less), including all values and ranges therebetween. In some embodiments, carbon coating 260 can have a thickness of about 500 nm, about 1 μm, about 2 μm, about 3 μm, about 4 μm, about 5 μm, about 6 μm, about 7 μm, about 8 μm, about 9 μm, about 10 μm, about 11 μm, about 12 μm, about 13 μm, about 14 μm, about 15 μm, about 16 μm, about 17 μm, about 18 μm, about 19 μm, or about 20 μm.

[0065] FIG. 3 is a diagram of an electrochemical cell 300 according to an embodiment. As shown, the electrochemical cell 300 includes a cathode 310 disposed on a cathode current collector 320, an anode 330 disposed on an anode current collector 340, a separator 350 disposed between the cathode 310 and the anode 330, and a carbon coating 360 disposed between the anode 330 and the separator 350. In some embodiments, the cathode 310, the cathode current collector 320, the anode 330, the anode current collector 340, the separator 350, and the carbon coating 360 can be the same as or substantially similar to the cathode 210, the cathode current collector 220, the anode 230, the anode current collector 240, the separator 250, and the carbon coating 260 described above with reference to FIG. 2. Accordingly, specific aspects of the cathode 310, the cathode current collector 320, the anode 330, the anode current collector 340, the separator 350, and the carbon coating 360 are not described in further detail herein.

[0066] In some embodiments, the anode 330 can have a thickness greater than the thickness of the cathode 310. In some embodiments, the ratio of the thickness of the anode 330 to the thickness of the cathode 310 can be at least about 1.1, at least about 1.2, at least about 1.3, at least about 1.4, at least about 1.5, at least about 1.6, at least about 1.7, at least about 1.8, at least about 1.9, at least about 2, at least about 2.5, at least about 3, at least about 3.5, at least about 4, at least about 4.5, at least about 5, at least about 5.5, at least about 6, at least about 6.5, at least about 7, at least about 7.5, at least about 8, at least about 8.5, at least about 9, or at least about 9.5. In some embodiments, the ratio of the thickness of the cathode 310 to the thickness of the anode 330 can be about 10 or less, about 9.5 or less, about 9 or less, about 8.5 or less, about 8 or less, about 7.5 or less, about 7 or less, about 6.5 or less, about 6 or less, about 5.5 or less, 5 or less, about 4.5 or less, about 4 or less, about 3.5 or less, about 3 or less, about 2.5 or less, about 2 or less, about 1.9 or less, about 1.8 or less, about 1.7 or less, about 1.6 or less, about 1.5 or less, about 1.4 or less, about 1.3 or less, about 1.2 or less. Combinations of the above thickness ratios are also possible (e.g., at least about 1.1 or more and about 10 or less, or at least about 3 or more and about 8 or less), including all values and ranges therebetween. In some embodiments, the ratio of the thickness of the anode 330 to the thickness of the cathode 310 can be about 1.1, about 1.2, about 1.3, about 1.4, about 1.5, about 1.6, about 1.7, about 1.8, about 1.9, about 2, about 2.5, about 3, about 3.5, about 4, about 4.5, about 5, about 5.5, about 6, about 6.5, about 7, about 7.5, about 8, about 8.5, about 9, about 9.5, or about 10.

[0067] Figures 4A - 4B are simulation plots of the performance of an electrochemical cell. Figure 4A shows the cell potential at various charging times during charging at 1.5C. Using COMSOL Multiphysics, rapid charging above 1C was simulated using a 3.0M electrolyte, an anode with a thickness of 190μm, a cathode with a thickness of 300μm, and a separator with a thickness of 12μm. Figure 4B shows the salt concentration profiles of the cathode, separator, and anode during 1.5C charging at different charging times. As shown in the figure, the spatial coordinate of 0.0005m corresponds to the interface between the anode and the current collector, and the spatial coordinate of 0m corresponds to the interface between the cathode and the current collector. Thus, the salt concentration is uniform throughout the electrode and becomes non - uniformly distributed during the charging of the electrochemical cell. Thus, at approximately 600s, the electrolyte salt concentration has an average gradient of approximately 2×10 8 mol / m 4 at t = 600s, approximately 2.9×10 8 mol / m 4 at t = 1200s, and approximately 2.6×10 8 mol / m 4 at t = 1800s.

Example

[0068] Figure 5 shows the density of an electrolyte containing LiFSI salt in a solvent with EC / DMC at 3:7 (w:w) and VC at 2wt%. The X - axis shows the molar concentration of the LiFSI salt in the solution. As shown in the figure, there is a strong linear correlation between the salt concentration and the density. The higher the salt concentration, the higher the density.

[0069] Figure 6 shows the rate capabilities when the orientation of the cell is changed. To utilize the density gradient within the cell, the influence of gravity on the rate capabilities was investigated. That is, the orientation of the electrochemical cell was changed to examine the difference in rate capabilities. The data indicated by the blue dots correspond to vertically oriented cells, and the length dimension of the electrodes is aligned with gravity. The data indicated by the orange dots correspond to horizontally oriented cells, and the thickness dimension of the electrodes is aligned with gravity, with the cathode at the top. The data indicated by the green dots correspond to horizontally oriented cells, with the anode at the top. As shown in the figure, horizontally oriented cells have better rate capabilities than vertically oriented cells. Cells with the cathode on top are hardly distinguishable from cells with the anode on top.

[0070] To evaluate the cause of the better rate capabilities of horizontally oriented cells, the capacity retention at 1.5C charge relative to the capacity at C / 10 charge and the area-specific impedance (ASI) relative to the internal resistance (IR) were compared. Figure 7 shows the general negative correlation of 1.5C capacity retention vs. IR and the positive correlation of 1.5C capacity retention vs. ASI. However, horizontally oriented cells showed a capacity retention about 20% higher at similar IR values compared to vertically oriented cells. This suggests that the orientation of the cell is important in rapid charging capabilities. The effect is not seen in the steady state before cycling but appears during charging when there is a concentration gradient in the electrolyte. Convection induced by gravity and the density difference of the electrolyte throughout the cell may at least partially improve the rapid charging capabilities of the cell when the concentration gradient and gravity are aligned in the same direction.

[0071] Figure 8 shows the rapid charging ability of an electrochemical cell using a 2M single salt. The electrolyte was formed from 2M LiFSI with EC / PC / EMC (2:1:7 wt%) + 0.5 wt% VC + 1.5 wt% DTD + 2 wt% TTE. The electrolyte was integrated into cells with 49 vol% LFP and 55 vol% LFP. The 49 vol% LFP cell contained Ketjen carbon, and the 55 vol% LFP cell contained PBX-51. Both cells contained an LFP anode with a thickness of 200 μm. The cathode included the HDL11 cathode. The cells were discharged at 1C or more to 0.8 SOC and charged at C / 4 to 1.0 SOC. The separator was made of polyethylene. As shown in the figure, both cells maintained more than 90% of their original capacity through 100 cycles.

[0072] Figure 9 shows the rapid charging ability of an electrochemical cell using a 2M dual salt. The electrolyte was formed from 1.5M LiPF6 and 0.5M LiFSI with EC / PC / EMC (2:1:7 wt%) + 0.5 wt% VC + 1.5 wt% DTD + 2 wt% TTE. The cell was discharged at 1C or more to 0.8 SOC and charged at C / 4 to 1.0 SOC. The electrolyte was incorporated into a cell with 49 vol% Ketjen added. This cell contained the HDL11 cathode and a polyethylene separator. As shown in the figure, this cell maintained more than 90% of its original capacity through 220 cycles.

[0073] Various concepts may be embodied in one or more ways, and at least one example of each is provided. The acts performed as part of the present methods may be ordered in any suitable manner. Accordingly, even though exemplary embodiments are shown as sequential acts, embodiments may be constructed in which some acts are performed concurrently, including in a different order than that shown, and still fall within the scope of the present disclosure. Stated another way, such features are not necessarily limited to a particular order of execution, but rather may be executed in serial, asynchronous, simultaneous, parallel, synchronous, and / or any number of threaded, processes, services, servers, and / or the like in a manner consistent with the present disclosure. Accordingly, some of these features may be mutually contradictory in that they cannot be present simultaneously in a single embodiment. Similarly, some features may be applicable to one aspect of the invention and not to others.

[0074] Furthermore, the present disclosure may include other inventions not presently described. Applicant reserves all rights in such inventions, including the right to practice such inventions and to file additional applications, continuations, continuation-in-parts, divisions, and / or the like. Thus, it should be understood that the advantages, embodiments, examples, functions, features, logical, operational, organizational, structural, topological, and / or other aspects of the present disclosure are not to be considered limitations of the present disclosure as defined by the embodiments or limitations of equivalents of the embodiments. Depending on the particular desires and / or characteristics of individual and / or corporate users, database configurations and / or relational models, data types, data transmissions and / or network frameworks, syntax structures, and the like, the various embodiments of the technology disclosed herein may be implemented in ways that provide great flexibility and customization as described herein.

[0075] All definitions, as defined and used herein, should be understood to take precedence over dictionary definitions, definitions in incorporated documents by reference, and / or ordinary meanings of defined terms.

[0076] As used herein, in certain embodiments, when preceding a numerical value, the term "about" or "approximately" indicates a range of plus or minus 10% of the value. When a range of values is provided, unless the context clearly indicates otherwise, each intervening value between the lower and upper limits of that range, to one-tenth of the unit of the lower limit, as well as any other stated value or intervening value within the stated range, is to be understood as being included within the present disclosure. The upper and lower limits of these smaller ranges may independently be included in the smaller ranges and are subject to any specifically excluded limit values of the stated range and are included within the present disclosure. When the stated range includes one or both of the limits, ranges excluding one or both of those included limits are also included in the present disclosure.

[0077] As used herein and in the present application in embodiments, the phrase "and / or" is to be understood to mean "either or both" of the elements so conjoined, i.e., elements that may exist conjunctively in some cases and disjunctively in other cases. A plurality of elements listed with "and / or" are to be construed in the same manner, i.e., as "one or more" of the elements so conjoined. Other elements may optionally exist, whether or not they are related to the specifically identified elements, other than those specifically identified by the "and / or" clause. Thus, by way of non-limiting example, reference to "A and / or B" can, when used in conjunction with open-ended language such as "comprising", in one embodiment, refer to only A (optionally including elements other than B), in another embodiment, refer to only B (optionally including elements other than A), and in yet another embodiment, refer to both A and B (optionally including other elements).

[0078] As used herein and in the claims of the present application, "or" should be understood to have the same meaning as "and / or" as defined above. For example, when separating items in a list, "or" or "and / or" is to be interpreted as inclusive, i.e., including at least one of the number of elements or the list, but more than one, and optionally including additional unlisted items. For example, only terms that are explicitly indicated to the contrary, such as "only one of" or "exactly one of", or when used in embodiments, "consisting of", will refer to the inclusion of exactly one element of the number of elements or the list. Generally, as used herein, the term "or" should be interpreted as indicating exclusive alternatives (i.e., "one or the other, but not both") only when preceded by an exclusive term such as "either", "one of", "only one of", or "exactly one of".

[0079] As used herein and in the claims of the present application, when referring to a list of one or more elements, the phrase "at least one" should be understood to mean at least one element selected from any one or more of the elements in the list of elements, but not necessarily specifically listed in the list of elements and not necessarily including at least one of each element that excludes any combination of the elements in the list of elements. This definition also allows for the possibility that elements other than those specifically identified in the list of elements referred to by the phrase "at least one" may optionally be present, whether or not they are related to the specifically identified elements. Thus, by way of non-limiting example, "at least one of A and B" (or equivalently, "at least one of A or B", or equivalently, "at least one of A and / or B") may, in one embodiment, include at least one, optionally two or more, of A and no B (and optionally include elements other than B); in another embodiment, include at least one, optionally two or more, of B and no A (and optionally include elements other than A); and in yet another embodiment, include at least one, optionally two or more, of A and at least one, optionally two or more, of B (and optionally include other elements), and so forth.

[0080] In embodiments and in the above specification, all transitional phrases such as "comprising", "including", "carrying", "having", "containing", "involving", "holding", "consisting of", etc. are to be understood to be open-ended, i.e., to mean "including but not limited to". As described in Section 2111.03 of the Manual of Patent Examining Procedure (MPEP) of the United States Patent and Trademark Office, only the transitional phrases "consisting of" and "consisting essentially of" must be closed or semi-closed transitional phrases, respectively.

[0081] While specific embodiments of the present disclosure have been outlined above, many alternatives, modifications, and variations will be apparent to those skilled in the art. Accordingly, the embodiments are intended to be illustrative rather than limiting, as described herein. Various changes may be made without departing from the spirit and scope of the present disclosure. If the methods and steps described above indicate certain events occurring in a particular order, those skilled in the art who benefit from the present disclosure may change the order of certain steps, and will recognize that such changes follow the variations of the invention. Further, some steps may not only be executed sequentially as described above, but also, if possible, simultaneously in parallel processing. Although the embodiments have been illustrated and described in detail, it is understood that various modifications in form and detail may be made.

Claims

1. An anode current collector, A semi-solid anode disposed on the anode current collector, wherein the anode current collector has a thickness of at least about 150 μm and includes an active material, a conductive material, and an electrolyte, and the electrolyte includes a non-aqueous solvent and an electrolyte salt, the semi-solid anode; A cathode current collector, A cathode disposed on the cathode current collector, A separator disposed between the cathode and the anode, comprising: Here, an electrochemical cell in which the electrolyte salt has an average concentration gradient in a semi-solid anode of at least about 2×10 ７ mol / m ４ .

2. The electrolyte salt has an average concentration in the non-aqueous liquid electrolyte of at least about 2,000 mol / m ３ of the electrochemical cell according to claim 1.

3. The electrolyte salt has an average concentration in the non-aqueous liquid electrolyte of at least about 3,000 mol / m ３ of the electrochemical cell according to claim 2.

4. The electrolyte salt has an average concentration gradient in the semi-solid anode of at least about 3×10 ７ mol / m ４ as claimed in claim 1, of the electrochemical cell.

5. The electrolyte salt contains at least one of lithium bis(oxalato)borate (LiBOB), lithium hexafluorophosphate (LiPF ６ ), or lithium bis(fluorosulfonyl)imide (LiFSI), and the electrochemical cell according to claim 1.

6. The electrochemical cell according to claim 1, wherein the separator is coated with the non-aqueous liquid electrolyte.

7. The electrochemical cell according to claim 6, wherein the separator is coated with hard carbon.

8. Combining an active material, a conductive material, and a non-aqueous electrolyte to form a semi-solid anode, the non-aqueous electrolyte having a salt concentration of at least about 2,000 mol / m3; Disposing the semi-solid anode on the anode current collector, the semi-solid anode having a thickness of at least about 150 μm; Disposing a cathode on the cathode current collector; Wetting a first surface of the separator with the non-aqueous electrolyte; Coating the first surface of the separator with carbon; Disposing the cathode on the anode with the separator interposed therebetween to form an electrochemical cell, such that the first surface of the separator contacts the semi-solid anode. A method comprising:

9. The method according to claim 8, further comprising charging and discharging the electrochemical cell while the electrochemical cell is oriented such that the thickness of the anode is aligned with the direction of gravity.

10. The method according to claim 8, wherein the non-aqueous liquid electrolyte has a salt concentration of at least about 3,000 mol / m ３ 2.

11. The method according to claim 8, wherein the carbon coating comprises hard carbon.

12. The method according to claim 9, wherein the charging and the discharging are performed at a rate of at least about 1.5 C.

13. The method according to claim 8, comprising charging and discharging the electrochemical cell while applying at least one of a magnetic field, heating, and centrifugal force to the electrochemical cell.

14. The method according to claim 8, wherein the first non-aqueous liquid electrolyte contains at least one of vinylene carbonate (VC), 1,3-propane sultone (PS), ethyl propionate (EP), 1,3-propanediol cyclic sulfate (PSA / TS), fluoroethylene carbonate (FEC), ethylene sulfite (ES), tris(2-ethylhexyl) phosphate (TOP), ethylene sulfate (DTD), ethyl acetate (EA), maleic anhydride (MA), ethylene carbonate (EC), propylene carbonate (PC), dimethyl carbonate (DMC), or ethyl methyl carbonate (EMC).

15. A first current source, A first electrode material disposed on the first current collector and having a semi-solid composition, the first electrode material having a thickness of at least about 150 μm and comprising an active material, a conductive material, an electrolyte salt, and an electrolyte solvent, the electrolyte salt having a concentration gradient of at least about 2×10 ７ mol / m ４ along the thickness of the first electrode material, the first electrode material; and A second current collector, A second electrode material disposed on the second current collector, A separator disposed between the first electrode material and the second electrode material, An electrochemical cell comprising a carbon coating disposed between the first electrode material and the separator.

16. The electrochemical cell according to claim 15, wherein the carbon coating contains at least one of hard carbon, disordered carbon, graphite, graphite-like carbon or non-graphite carbon, amorphous carbon, mesophase carbon, spherulite, soft carbon, activated carbon, or a graphite-like hard carbon mixture.

17. The electrochemical cell according to claim 15, wherein the electrolyte solvent is a non-aqueous solvent.

18. The electrolyte salt has a concentration gradient along the thickness of the first electrode material of at least about 3×10 ７ mol / m ４ The electrochemical cell according to claim 15.

19. The electrolyte salt contains at least one of lithium bis(oxalato)borate (LiBOB), lithium hexafluorophosphate (LiPF ６ ), or lithium bis(fluorosulfonyl)imide (LiFSI). The electrochemical cell according to claim 15.

20. The first electrode has a viscosity gradient of at least about 5×10 ５ Pa·s / m, the electrochemical cell according to claim 15.

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