Method and system for upcycling used batteries

Abstract

The present disclosure provides methods and systems for recycling and upcycling spent battery cathode material. In some embodiments, the methods may include separating the spent battery cathode material into a plurality of particle populations, where a first population of the plurality of particle populations includes first particles of a first size and a second population of the plurality of particle populations includes second particles of a second size. The methods further include generating a first precursor solution using the first population of particles, generating a second precursor solution using the second population of particles, generating the first cathode material using the first precursor solution, and generating the second cathode material using the second precursor solution.

Description

[Technical Field]

[0001] CROSS-REFERENCE TO RELATED APPLICATIONS This application claims the benefit of U.S. Provisional Patent Application No. 63 / 374,569, entitled "METHOD AND APPARATUS FOR BATTERY CATHODE MATERIALS UPCYCLING," filed September 5, 2022, which is incorporated by reference herein in its entirety.

[0002] STATEMENT REGARDING FEDERALLY FUNDED RESEARCH This invention was made with government support under Grant DE-SC0020868 awarded by the Department of Energy. The government has certain rights in this invention.

[0003] This application relates generally to battery recycling, and more specifically to upcycling spent battery materials. [Background technology]

[0004] Lithium-ion batteries (LIBs) are widely used in many electrical devices, vehicles, and other applications. Used LIBs can pose environmental challenges and resource waste. End-of-life (EoL) LIBs are set to become an important secondary source of materials used in the production of new batteries. By reducing recycling costs and increasing recycling rates, the life cycle cost of LIBs can be significantly reduced. This reduction can also prevent material shortages, mitigate the environmental impact of producing new materials, and provide low-cost active materials for the production of new LIBs. With a predicted surge in cell production over the next decade, primary scrap from production is emerging as a significant source for global recycling efforts. Currently, the industry primarily relies on pyrometallurgical or hydrometallurgical methods to recycle LIBs. These methods are often followed by acid leaching or alkaline treatment processes to recover valuable elements such as Li, Ni, and Co. However, reliance on high temperatures and intensive chemical processes results in significant energy consumption, the generation of new chemical waste, and high operating costs. Innovative recycling technologies are essential to make LIB recycling profitable and stimulate industry expansion without imposing disposal fees on consumers. Direct recycling, which involves the recovery and reuse of battery components without changing their chemical structure, offers a route to providing battery manufacturers with more affordable reconstituted materials. This approach could potentially reduce the cost of electric vehicle (EV) batteries and therefore increase the attractiveness of recycling them.

[0005] Direct recycling of LIBs has gained attention as a viable method. Direct recycling of LIBs allows for the regeneration of cathode and anode materials without destroying their compounds, substantially reducing energy and chemical usage. However, a challenge lies in the age difference between recovered and modern materials. Recycled electrode materials are typically 5–10 years old and may not be aligned with evolving market demands, given advances in electrode material properties and the emergence of novel chemistries.

[0006] The development of effective upcycling processes that recover high-value forms of materials for resale to manufacturers is crucial to facilitating LIB recycling. A profitability-driven upcycling platform can align with market goals, including reducing battery costs and increasing the incorporation of recycled battery materials.

[0007] During long cycles, LiNi x Co y Mn z O2(NCM) and LiNi x Co y Al zMany particles in cathode materials, such as O2(NCA) (where x + y + z = 1), often collapse into primary nanoparticles. This loss of secondary structure amplifies the exposure of new surfaces to the electrolyte, leading to material degradation and subsequent loss of electrochemical performance. This degradation complicates full recovery of electrochemical performance in standard hydrothermal or high-temperature relithiation processes, which often cannot counteract the collapse of these nanoparticles. Summary of the Invention

[0008] The following is a simplified summary of the disclosure to provide a basic understanding of some aspects of the disclosure. This summary is not an extensive overview of the disclosure. It is not intended to identify key elements of the disclosure or to delineate the scope of particular implementations of the disclosure or the scope of the claims. Its sole purpose is to present some concepts of the disclosure in a simplified form as a prelude to the more detailed description that is presented later.

[0009] According to one or more aspects of the present disclosure, there is provided a method for upcycling spent batteries, the method including separating a cathode material of the spent batteries into a plurality of particle populations, wherein a first population of the plurality of particle populations includes first particles of a first size and a second population of the plurality of particle populations includes second particles of a second size, using the first particles to form a first precursor solution, using the second particles to form a second precursor solution, using the first precursor solution to form a first cathode material, and using the second precursor solution to form a second cathode material.

[0010] In some embodiments, the first particle is a microparticle and the second particle is a nanoparticle.

[0011] In some embodiments, the first precursor solution comprises at least one of a suspension containing the first group of particles or a solution containing the first group of particles.

[0012] In some embodiments, the first precursor solution is selected from the group consisting of LiOH, LiNO, LiAc, Ni(NO), Mn(NO), Co(NO), CHONi, Ni(Ac), CHOMn, Mn(Ac), C 12 H 10 MnO 14 , C2H2O4Co, Co(Ac)2, Al(NO3)3.

[0013] In some embodiments, the first precursor solution further comprises a lithium precursor.

[0014] In some embodiments, the first precursor solution includes at least one dopant precursor.

[0015] In some embodiments, producing the first cathode material using the first precursor solution includes calcining the first precursor solution to produce first calcined particles, and performing surface engineering on the first calcined particles.

[0016] In some embodiments, producing the second cathode material using the second precursor solution includes forming a plurality of microparticles using the second precursor solution and calcining the plurality of microparticles to produce second calcined particles.

[0017] In some embodiments, forming the plurality of microparticles using the second precursor solution comprises generating micronized droplets using at least one of a spray granulation process or a spray drying process.

[0018] In some embodiments, producing the second cathode material using the second precursor solution further includes performing surface engineering on the second calcined particles.

[0019] In some embodiments, the second precursor solution comprises at least one of a suspension containing the second group of particles or a solution containing the second group of particles.

[0020] In some embodiments, the second precursor solution is selected from the group consisting of LiOH, LiNO, LiAc, Ni(NO), Mn(NO), Co(NO), CHONi, Ni(Ac), CHOMn, Mn(Ac), C 12 H 10 MnO 14 , C2H2O4Co, Co(Ac)2, or Al(NO3)3.

[0021] In some embodiments, the second precursor solution comprises a Li precursor, the Li precursor comprising at least one of LiOH, LiNO 3 , and LiAc.

[0022] In some embodiments, the second precursor solution comprises a Mn precursor, the Mn precursor being selected from the group consisting of Mn(Ac), Mn(NO), CHO, Mn, C 12 H 10 MnO 14 or Mn(NO2)2.

[0023] In some embodiments, the second precursor solution includes a Co precursor, the Co precursor including at least one of Co(Ac)2, Co(NO3)2, C2H2O4CO, Co(NO2)2.

[0024] In some embodiments, the second precursor solution includes an Al precursor, and the Al precursor includes at least one of Al[OCH(CH)], Al(N(CH), Al[OCH(CH)CH], (CH)Al, and Al(NO).

[0025] In some embodiments, the second precursor solution comprises one or more dopant precursors, wherein the dopant precursors comprise at least one of Al, Ti, Mg, Ca, Nb, Zr, W, Te, Mo, or F.

[0026] According to one or more aspects of the present disclosure, a system for upcycling spent batteries is provided. The system may include: a particle separator configured to separate a cathode material of the spent battery into a plurality of particle groups, a first group of the plurality of particle groups including first particles of a first size and a second group of the plurality of particle groups including second particles of a second size; a precursor generator configured to generate a first precursor solution using the first particles and generate a second precursor solution using the second particles; and battery upgrade components configured to generate a first cathode material using the first precursor solution and generate a second cathode material using the second precursor solution.

[0027] In some embodiments, the first particle is a microparticle. In some embodiments, the second particle is a nanoparticle.

[0028] In some embodiments, the battery upgrade component further includes a calcination component configured to calcinate the first precursor solution to produce first calcined particles, and a surface engineering component configured to perform surface engineering on the first calcined particles.

[0029] In some embodiments, the battery upgrading component further includes a microparticle modifying component configured to form a plurality of microparticles using the second precursor solution.

[0030] The present disclosure will be more fully understood from the detailed description given below and from the accompanying drawings of various embodiments of the present disclosure, which should not be construed as limiting the disclosure to particular embodiments, but are for purposes of illustration and understanding. [Brief explanation of the drawings]

[0031] [Figure 1] FIG. 1 is a schematic diagram illustrating an exemplary system for upcycling spent batteries.

[0032] [Figure 2] FIG. 2 is a block diagram illustrating an exemplary process for producing cathode materials according to some embodiments of the present disclosure.

[0033] [Figure 3A] FIG. 3A illustrates an exemplary process for upcycling cathode materials according to some embodiments of the present disclosure. [Figure 3B] FIG. 3B illustrates an exemplary process for upcycling cathode materials according to some embodiments of the present disclosure.

[0034] [Figure 4] FIG. 4 is a schematic diagram illustrating an exemplary microparticle production reactor according to some embodiments of the present disclosure. [Figure 5] FIG. 5 is a schematic diagram illustrating an exemplary microparticle production reactor according to some embodiments of the present disclosure.

[0035] [Figure 6] FIG. 6 illustrates an exemplary baking system according to some embodiments of the present disclosure.

[0036] [Figure 7] FIG. 7 illustrates an exemplary surface engineered reactor according to some embodiments of the present disclosure.

[0037] [Figure 8A] FIG. 8A is a flowchart illustrating an exemplary process for upcycling spent batteries according to some embodiments of the present disclosure. [Figure 8B]FIG. 8B is a flowchart illustrating an exemplary process for upcycling spent batteries according to some embodiments of the present disclosure. [Figure 8C] FIG. 8C is a flowchart illustrating an exemplary process for upcycling spent batteries according to some embodiments of the present disclosure.

[0038] [Figure 9A] FIG. 9A is an SEM image of aged NCA cathode material.

[0039] [Figure 9B] FIG. 9B is an SEM image of the isolated damaged nanoparticles.

[0040] [Figure 9C] FIG. 9C is an SEM image of morphology-upgraded microparticles of upcycled NCA cathode material.

[0041] [Figure 9D] FIG. 9D shows the cycling performance of the upcycled NCA cathode material of FIG. 9C and the commercial NCA cathode material.

[0042] [Figure 10A] FIG. 10A shows the XRD pattern comparison between recycled polycrystalline NCM111 cathode material and upcycled single-crystalline NCM622 cathode material.

[0043] [Figure 10B] FIG. 10B is an SEM image of single-crystal NCM622 cathode material upcycled from spent polycrystalline NCM111 cathode material.

[0044] [Figure 10C] FIG. 10C shows the first cycle charge-discharge curves of the commercial polycrystalline NCM622 cathode material and the upcycled single-crystalline NCM622 cathode material at 0.1 C.

[0045] [Figure 10D] FIG. 10D shows a comparison of the cycling performance of upcycled single-crystalline NCM622 cathode material and commercial polycrystalline NCM622 cathode material at 1C.

[0046] [Figure 11A] FIG. 11A is an SEM image of spent LFP nanoparticles.

[0047] [Figure 11B] FIG. 11B is an SEM image of the morphology-upgraded LFP cathode material.

[0048] [Figure 11C] FIG. 11C shows the particle size distribution of the upgraded LFP cathode material.

[0049] [Figure 11D] FIG. 11D shows a comparison of the cycling performance of spent LFP nanoparticle and upgraded LFP microparticle cathode materials.

[0050] [Figure 12A] FIG. 12A is an SEM image of morphology and chemistry upgraded LMFP microparticle cathode material.

[0051] [Figure 12B] FIG. 12B depicts the particle size distribution of the upgraded LMFP cathode material.

[0052] [Figure 12C] FIG. 12C shows the XRD of the upcycled LFP microparticle cathode material and the LMFP microparticle cathode material.

[0053] [Figure 12D] FIG. 12D shows the second cycle charge-discharge curves of the upcycled LFP and LMFP cathode materials. DETAILED DESCRIPTION OF THE INVENTION

[0054] The present disclosure provides mechanisms (e.g., systems, devices, methods, etc.) for upcycling used batteries. As referred to herein, a battery may be any power storage device. In some embodiments, the battery may be a lithium-ion battery (LIB). Used batteries may include used and / or aged LIBs, battery modules, battery packs, etc. As used herein, "lithium-ion battery cathode material" refers to materials that make up the cathode of a LIB, including, but not limited to, lithium cobalt oxide, lithium nickel cobalt manganese oxide, lithium nickel cobalt aluminum oxide, lithium nickel cobalt manganese aluminum oxide, lithium manganese oxide, lithium iron phosphate, and lithium manganese iron phosphate.

[0055] Recycling LIBs can involve discharging spent LIBs and separating the spent graphite using physical methods such as dismantling, crushing, sieving, and other mechanical processes. The separated raw graphite anode material can be processed to produce recycled anode materials (e.g., by direct regeneration of graphite) and / or upcycled anode materials (e.g., by upgrading the graphite anode material to a graphite-based material with additional functionality desirable for energy and environmental applications). However, raw cathode materials obtained by separating them from other components of spent batteries may not meet battery industry standards due to impurities and structural defects.

[0056] According to one or more aspects of the present disclosure, a system for battery upcycling is provided. The system may process used batteries and produce refurbished and / or upgraded cathode material that can be used in electrodes of new batteries. For example, the system may process raw cathode material from used batteries (e.g., used and / or damaged LIB cathode material) and classify the cathode particles in the raw cathode material by size and / or morphology. In particular, the system may separate cathode particles having a desired size, morphology, and crystallinity (also referred to as "perfect cathode particles") from cathode particles lacking the desired size, morphology, and / or crystallinity (also referred to as "damaged cathode particles"). In some embodiments, the perfect cathode particles may include microparticles (e.g., particles with dimensions between 1 μm and 300 μm). The damaged cathode particles may include nanoparticles (e.g., particles with dimensions between 1 nm and 1000 nm).

[0057] The system may produce upcycled cathode materials by processing isolated intact microparticles and damaged nanoparticles. For example, intact cathode particles may undergo a regeneration and then a surface coating process to enhance their stability. Damaged nanoparticles may be processed for morphological reconstruction and enhancement. Larger particles (e.g., particles with dimensions of 1-100 microns) may be generated from damaged and disintegrated particles in a morphological recovery process involving the formation of a nanoparticle suspension or solution with modified chemical composition and / or additional dopants, followed by rapid gas-phase processing to form new particles with upgraded chemistry at low temperatures. Additionally, nanoprecursors may be used as seeds for the synthesis of even larger single-crystalline particles.

[0058] Recycled cathode materials produced using the mechanisms described herein can exhibit desired morphology, composition, dopants, and crystallinity. The ability of the upcycled cathode materials can match that of virgin cathode materials suitable for fabricating new battery (e.g., LIB) electrodes. Recycled cathode materials can include, for example, morphology-upgraded lithium-ion battery cathode particles, chemistry-upgraded LIB cathode particles, desired dopants, crystalline structure-upgraded LIB cathode particles, etc.

[0059] By rapidly separating particles and efficiently repairing damaged cathode particles, excellent cathode yields (95%-98%) can be achieved. Excellent cathode yields are achieved with substantially less energy than traditional energy-intensive cathode resynthesis from dissolved salt precursors. Such efficiencies could significantly increase the adoption rate of LIB recycling and regeneration processes. Furthermore, these regenerated materials could be increasingly utilized in EVs, stationary energy storage solutions, and consumer electronics.

[0060] As used herein, "desired morphology" can refer to a predetermined morphological characteristic of a particle. In some cases, the desired morphology is a desired shape and / or a desired size. In some cases, the desired morphology is substantially spherical.

[0061] As used herein, "desired crystallinity" or "desired crystal structure" may refer to a predetermined crystalline structure of a particle, which may be conventionally measured by X-ray diffraction (XRD) or another method capable of providing similar information. In some cases, the desired crystallinity described herein is a layered structure with hexagonal symmetry belonging to the space group R-3m (e.g., for NCM, NCA, and NCMA chemistries). In some embodiments, the desired crystallinity is an ilmenite-derived structure belonging to the orthorhombic Pnma space group (e.g., for LFP and LMFP chemistries). As used herein, "morphology-upgraded lithium ion battery cathode particles" may refer to lithium ion battery cathode particles whose morphology and / or particle size (e.g., nanoparticles) have been adjusted. For example, the nanoparticles used in NCA lithium ion battery cathode particles and LFP lithium ion battery cathode particles may be upgraded by morphology modification to microsphere-like lithium ion battery cathode particles.

[0062] As used herein, "chemically upgraded lithium-ion battery cathode particles" can refer to lithium-ion battery cathode particles in which the stoichiometry of lithium and other elements has been adjusted. For example, the stoichiometry of NCM523 lithium-ion battery cathode particles can be adjusted by adding more Li, Ni, and Co precursors, such that NCM523 lithium-ion battery cathode particles are upgraded to NCM811 lithium-ion battery cathode particles. The stoichiometry of LFP lithium-ion battery cathode particles can be adjusted by adding more Li, Mn, and P precursors, such that LFP lithium-ion battery cathode particles are upgraded to LMFP lithium-ion battery cathode particles.

[0063] As used herein, "crystalline structure-upgraded lithium-ion battery cathode particles" can refer to lithium-ion battery cathode particles whose crystalline structure has been adjusted. For example, polycrystalline NCM111 lithium-ion battery cathode particles can be adjusted by applying a second calcination process such that the polycrystalline NCM111 lithium-ion battery cathode particles are upgraded to NCM111 single-crystalline lithium-ion battery cathode particles.

[0064] As used herein, "NCM" refers to lithium nickel cobalt manganese oxide; "NCA" refers to lithium nickel cobalt aluminum oxide; "NCMA" refers to lithium nickel cobalt manganese aluminum oxide; "LFP" refers to lithium iron phosphate; and "LMFP" refers to lithium manganese iron phosphate.

[0065] 1 is a schematic diagram illustrating an exemplary system 100 for upcycling used batteries. The used batteries may include, for example, used and / or damaged LIBs.

[0066] As shown, system 100 may include a pre-treatment component 110, a particle separator 120, a precursor generator 130, a microparticle modification component 140, a calcination component 150, a surface engineering component 160, and / or any other suitable components for upcycling spent batteries in accordance with the techniques described herein. The microparticle modification component 140, the baking component 150, and the surface engineering component 160 may be collectively referred to as the battery upgrade component 170. System 100 may include more or fewer modules without loss of generality. For example, two of the components may be combined into a single component, or one of the components may be split into two or more components.

[0067] The pretreatment component 110 may process the raw cathode material of the spent batteries using aqueous methods to produce pretreated raw cathode material 115. The raw cathode material may be collected from spent batteries, for example, by discharging the batteries and separating the raw cathode material using a mechanical process (e.g., disassembly, crushing, sieving, etc.). In some embodiments, the spent batteries may exhibit the same chemical type (e.g., contain the same cathode material). The raw cathode material may include, for example, lithium nickel cobalt manganese oxide, lithium nickel cobalt aluminum oxide, lithium nickel cobalt manganese aluminum oxide, lithium iron phosphate, lithium iron manganese phosphate, etc.

[0068] In some embodiments, the pretreatment component 110 may purify the raw cathode material by flowing a fluidized gas-solids stream of the particle mixture and exposing the flowing particle mixture through a plasma region to a non-equilibrium plasma, which may have a predetermined power density and a predetermined solid-to-gas volume ratio for a predetermined exposure time to remove impurities.

[0069] The particle separator 120 may separate the pretreated cathode material 115 (e.g., purified cathode material) into multiple particle groups of various sizes and / or morphologies. Each group may have particles of a specific size and / or size distribution. For example, the pretreated cathode material 115 may be divided into a first particle group 125a and a second particle group 125b. The first particle group 125a may have a desired morphology and / or a desired particle size. The second particle group 125b lacks the desired morphology or size of the first group. More specifically, for example, the first particles 125a may have a desired shape and / or size and may include perfectly spherical microparticles of about 1 to about 100 μm. The second particles 125b lack such a morphology or size and may include nanoparticles of about 1 nm to about 1000 nm.

[0070] Separation of the first and second particle groups can be achieved in a gas-phase centrifugation process by controlling the gas pressure and aerodynamic characteristics of the gas flow. In some embodiments, the particle separator 120 may separate the pretreated cathode material 115 into particle groups using gas-phase centrifugal forces in a vortex motion. In some embodiments, the particle separator 120 may include an axial cyclone separator combined with a swirling gas under a non-equilibrium and low-temperature plasma discharge. The axial cyclone separator may utilize rapid particle separation in the gas phase, directly and selectively selecting intact cathode particles. Separation of intact and damaged cathode particles may reduce the steps and costs for recycling and upcycling cathode materials.

[0071] The precursor generator 130 may generate one or more precursor solutions using the first particles 125a and / or the second particles 125b. In some embodiments, the precursor solution may include particles 125a and / or particles 125b, a solvent, a binder, etc., to form a suspension and / or solution including one or more chemistry-adjusting additives and one or more dopant precursors. The incorporation of small amounts (0.01-5%) of dopants occupying transition metal (TM) sites or Li sites or oxygen sites within the cathode structure may improve the structural and electrochemical properties of the initial cathode material.

[0072] The chemistry modifying additive may include chemicals containing Ni, Mn, Co, P, or Li that are used to change the stoichiometry of each element in the lithium ion battery cathode material (e.g., NCM, NCA, NCMA, LFP, LMFP) upon contact with the particles of the lithium ion battery cathode material used. Examples of chemistry modifying additives include LiOH, LiNO3, LiAc, Ni(NO3)2, Mn(NO3)2, Co(NO3)2, C2H2O4Ni, Ni(Ac)2, C2H2O4Mn, Mn(Ac)2, C 12 H 10 MnO 14, C2H2O4Co, Co(Ac)2, Al(NO3)3, Al[OCH(CH3)2]3, Al(N(CH3)2)3, Al[OCH(CH3)C2H5]3, (CH3)3Al, etc.

[0073] Doping additives may include chemicals containing Al, Ti, Mg, Ca, Nb, Zr, W, Te, Mo, F, etc., instead of Ni, Co, Mn, or oxygen (O). Doping strategies can play an important role in improving the structural and electrochemical properties of initial cathode materials (e.g., NCMs) in which dopants occupy transition metal (TM) sites, Li sites, or oxygen sites within a layered cathode structure with a space group of R-3m. The incorporation of small amounts of one or more doping elements is effective in mitigating the volume change of layered cathodes during phase transitions under high-voltage conditions. Meanwhile, the addition of one or more doping elements to the Li sites acts as pillars, improving rate performance and structural stability during cycling. Additionally, the addition of one or more doping elements to the Li sites can increase the energy density of the cathode material through the oxidation and / or reduction of oxygen. Solvents can include, for example, water, ethanol, methanol, isopropanol, ethylene glycol, etc. The organic binder may include, for example, polyethylene glycol (PEG), polyvinyl alcohol (PVA), polyvinyl butyral (PVB), and the like.

[0074] As an example, the precursor generator 130 may use the first particles 125a to generate a first precursor solution 135a. The first precursor solution 135a may further include a solvent, a binder, one or more chemistry-adjusting additives, one or more dopant precursors, etc. As another example, the precursor generator 130 may use the second particles 125b to generate one or more second precursor solutions 135b. Each of the second precursor solutions 135b may further include a solvent, a binder, one or more chemistry-adjusting additives, one or more dopant precursors, etc. The solvent may include, for example, water, ethanol, methanol, isopropanol, ethylene glycol, etc. The organic binder may include, for example, PEG, PVA, PVB, etc. The chemistry-adjusting additive may include a lithium (Li) precursor, a manganese (Mn) precursor, a nickel (Ni) precursor, a carbon (Co) precursor, an aluminum (Al) precursor, one or more dopant precursors, etc. Li precursors may include, for example, LiOH, LiNO3, LiAc, etc. Examples of Ni precursors may include Ni(Ac)2, Ni(NO3)2, C2H2O4Ni, NiBr2, etc. Examples of Mn precursors may include Mn(Ac)2, Mn(NO3)2, C2H2O4Mn, C 12 H 10 MnO 14 , Mn(NO) and the like. Examples of Co precursors may include Co(Ac), Co(NO), CHOCo, Co(NO), and the like. Examples of Al precursors may include Al[OCH(CH)], Al(N(CH), Al[OCH(CH)CH], (CH)Al, Al(NO), and the like. Dopant precursors may include chemicals containing Al, Ti, Mg, Ca, Nb, Zr, W, Te, Mo, or F in place of Ni, Co, Mn, or oxygen (O), and the like. In some embodiments, the first precursor solution 135a may include precursor solution 210, as described in connection with FIG. 2. In some embodiments, the second precursor solution 135b may include another precursor solution 220, 230, 240, and 250, as described in connection with FIG. 2.

[0075] The microparticle modification component 140 may use the second precursor solution 135b to produce microparticles 145. The microparticles may have a preferred size of 1 μm to 100 μm. For example, the microparticle modification component 140 may perform precursor powder synthesis via a droplet generation process. In some embodiments, the droplet generation process may involve utilizing a spray granulation process and / or a spray drying process to produce finely divided droplets. In some embodiments, the spray drying process and / or the spray granulation process may involve droplet generation and drying of a suspension or solution comprising a solution of the Li precursor in which the particles are suspended.

[0076] In some embodiments, the atomized droplets may be generated utilizing a centrifugal droplet generation process, which may involve generating droplets using artificial gravity.

[0077] In some embodiments, spray drying or spray granulation can be adjusted to produce agglomerates having a suitable size between 1 μm and 100 μm. For example, spray drying or spray granulation can be adjusted to produce droplets of a given size, which are then dried into agglomerates of the desired size. In some embodiments, the droplet generator can be and / or include a centrifugal atomizer or a gas atomizer to produce droplets of the desired size (e.g., by adjusting nozzle design, liquid selection, air flow, reactor design, etc.).

[0078] In some embodiments, the spray-drying or spray-granulation reactor may use a drying gas to evaporate the liquid at 50° C. to 400° C. The drying gas may be and / or may include, for example, air, O2, N2, Ar, etc. In some embodiments, the dried microparticles have a desired morphology and may be spherical or substantially spherical.

[0079] In some embodiments, the microparticle modification component 140 may include a microparticle production reactor 400 as described in connection with FIG. 4 and / or a microparticle production reactor 500 as described in connection with FIG. 5.

[0080] The calcination component 150 may calcinate the first particles 125a to produce the first calcined particles 155a and the microparticles 145 in situ. Calcination of the first particles 125a may allow for relithiation of the first particles 125a, producing the first calcined particles 155a. Calcination of the microparticles 145 may achieve relithiation, metal restoration, doping, crystallization, etc., of the microparticles 145, producing the second calcined particles 155b. For example, the calcination component 150 may calcinate the first particles 125a and / or the microparticles 145 by ebullated bed pre-calcination and warm plasma calcination. In the ebullated bed pre-calcination process, a first high temperature causes decomposition of the precursor compounds within the microparticles into oxides, which forms strong bonds to bind any small nanoparticles within the particles together and prevent agglomeration due to incomplete decomposition of the precursors. In the plasma sintering process, a second elevated temperature from an internal plasma discharge is applied to the pre-sintered particles to form sintered particles having the desired crystallinity.

[0081] In some embodiments, the firing component 150 may apply a first elevated temperature to the first group of particles 125a for pre-firing, and in some embodiments, the firing component 150 may apply a plasma at a second elevated temperature for additional firing.

[0082] In some embodiments, the first elevated temperature and residence time of the particles in the ebullated bed chamber provides control over particle porosity and morphology. The second elevated temperature and temperature profile along the particle flow path in this in-line plasma sintering zone can be controlled by various parameters to achieve the desired cathode material.

[0083] In some embodiments, the first elevated temperature in the ebullated bed is a temperature between 200° C. and 700° C. In some embodiments, the second elevated temperature in the plasma reactor is a temperature between 600° C. and 2000° C.

[0084] In some embodiments, the firing component 150 may perform an additional firing process to upgrade the fired particles from a polycrystalline phase to a single crystalline phase. In some embodiments, the additional firing process may be performed in a chamber with or without a plasma.

[0085] In some embodiments, the baking component 150 can include a baking system 600, as described in connection with FIG.

[0086] The surface engineering component 160 may perform surface engineering on the first calcined particles 155 a and the second calcined particles 155 b for relithiation, restoration, crystallization, carbon coating, and / or modification of the calcined particles. The surface engineering component 160 may produce a first cathode material 165 a by treating the first calcined particles 155 a, and a second cathode material 165 b by treating the second calcined particles 155 b. The first cathode material 165 a and the second cathode material 165 b may be battery-grade cathode materials that can be used to fabricate cathode electrodes for new batteries.

[0087] In some embodiments, the surface engineering component 160 may utilize a fluidized bed spray coating process to perform the surface engineering process. The coating process may be adapted from existing batch-based state-of-the-art methods for battery recycling to facilitate continuous flow operation. When a solution or suspension is used for coating, the liquid may act to transport the solids of the coating agent (also called precursor) to the particle surface. Fluidized bed spray coating may involve depositing a precursor on the first calcined particles 155a and / or the second calcined particles 155b, followed by calcination in a second ebullated bed. The coating precursor may include a mixture of one or more coating agents, a solvent, a binder, etc. Coating agents may include, for example, carbon, LiF, Al2O3, TiO2, ZrO2, Li3PO4, LiNbO2, etc. Example solvents may include water, ethanol, methanol, isopropanol, ethylene glycol, etc. In some embodiments, the binder may include, for example, PEG, PVA, PVB, etc. The surface engineering component 160 may, in some embodiments, include a surface engineering reactor 700, as described in connection with FIG.

[0088] FIG. 2 is a block diagram 200 illustrating an exemplary process for producing cathode materials according to some embodiments of the present disclosure.

[0089] In some embodiments, precursor solution 210 may be processed by in-line firing component 150 and surface engineering component 160 of FIG. 1 for surface coating. Precursor solution 210 may include first particles 125a, a solvent, a binder, one or more lithium precursors, one or more dopant precursors, etc. Processing of precursor solution 210 may produce cathode material 210a.

[0090] In some embodiments, precursor solution 220 may be processed by microparticle modification component 140, in-line calcination component 150, and surface engineering component 160 of FIG. 1 for morphology modification. Precursor solution 220 may include second particles, a solvent, a binder, one or more lithium precursors, one or more chemistry-adjusting additives, one or more dopant precursors, etc. Processing of precursor solution 220 may produce cathode material 220a.

[0091] In some embodiments, the precursor solution 230 may be processed by a microparticle modification component 140, a calcination component 150, and a surface engineering component for chemical upgrade. The precursor solution 230 may include second particles 125b, a solvent, a binder, one or more lithium precursors, one or more chemistry adjusting additives, one or more dopant precursors, etc. Processing of the precursor solution 230 may produce a cathode material 230a.

[0092] In some embodiments, the precursor solution 240 may be processed by the microparticle modification component 140 and the in-line calcination component 150 for crystal structure upgrading. For example, the microparticle modification component 140 may use the precursor solution 240 to produce microparticles. The microparticles may then be calcined by the calcination component 150 of FIG. 1 . An additional calcination process may be performed on the calcined microparticles to produce the cathode material 240a. The precursor solution 240 may include the second particles 125b, a solvent, a binder, one or more lithium precursors, etc. The precursor solution 240 may or may not contain a chemistry-adjusting additive. The precursor solution 240 may or may not contain a dopant precursor.

[0093] In some embodiments, precursor solution 250 may be processed by microparticle modification component 140, calcination component 150, and surface engineering component 160 to produce cathode material 250a. Precursor solution 250 may include second particles 125b, metal leachates, solvents, binders, lithium precursors with chemistry-adjusting additives, etc. Precursor solution 250 may include one or more of Ni precursors, Mn precursors, Co precursors, Li precursors, dopant precursors, etc.

[0094] 3A and 3B are diagrams illustrating exemplary particles of cathode material according to some embodiments of the present disclosure.

[0095] As shown in FIG. 3A , the raw cathode material 105 can be purified (e.g., by the pretreatment component 110 of FIG. 1 ) and separated into first particles 125 a and second particles 125 b (e.g., by the particle separator 120 of FIG. 1 ). The calcined first particles 155 a can be produced by relithiation and calcination of the first particles 125 a (e.g., by the precursor generator 130 and calcination component 150 of FIG. 1 ). The first cathode material 165 a can be produced by performing surface engineering (e.g., surface coating) on ​​the calcined first particles 155 a (e.g., by the surface engineering component 160 of FIG. 1 ). The first particles 125 a can be regenerated in a subsequent relithiation step.

[0096] The size of the second particles 125b is typically in the range of 50-1000 nanometers. As described in more detail below, the second particles 125b can be restored to larger particles (5-15 microns) in a morphology recovery process that involves only the formation of a nanoparticle suspension in water followed by rapid gas-phase processing at low temperatures of 40-400°C.

[0097] By combining rapid particle separation with rapid restoration of damaged particles, high overall cathode yields (95%-98%) can be achieved with much lower energy consumption compared to the energy-intensive cathode resynthesis process from dissolved salt precursors. This will significantly accelerate the market penetration of LIB recycling and regeneration as well as the use of recycled materials for EVs and stationary energy storage.

[0098] Referring to FIG. 3B , microparticles 345a may be produced by adding one or more Li precursors, C precursors, and dopant precursors to second particles 125b and upgrading the morphology of second particles 125b (e.g., using precursor generator 130 and microparticle modification component 140 of FIG. 1 ). Calcined particles 355a may be produced by calcining microparticles 345a using calcination component 150 of FIG. 1 . Calcining microparticles 345a may achieve relithiation, elemental doping, and carbon coating of microparticles 345a. Upcycled cathode material 365a may be produced by performing surface engineering (e.g., surface coating) on ​​calcined particles 355a (e.g., by surface engineering component 160 of FIG. 1 ).

[0099] Microparticles 345b may be produced by adding one or more Li precursors and one or more dopant precursors, M precursors, P precursors, C precursors, etc. to second particles 125b to upgrade the morphology and chemical properties of second particles 125b (e.g., by the precursor generator 130 and microparticle modification component 140 of FIG. 1 ). Calcined particles 355b may be produced by calcining microparticles 345b using the calcination component 150 of FIG. 1 . Calcining microparticles 345b may achieve relithiation, metal restoration, and carbon coating of microparticles 345b. Upcycled cathode material 365b may be produced by performing surface engineering (e.g., surface coating) on ​​calcined particles 355b (e.g., by the surface engineering component 160 of FIG. 1 ).

[0100] Microparticles 345c may be produced by adding one or more Li precursors, M precursors, etc. to second particles 125b and modifying second particles 125b (e.g., using precursor generator 130 and microparticle modification component 140 of FIG. 1 ). Calcined particles 355c may be produced by calcining microparticles 345c using calcination component 150 of FIG. 1 . Calcining microparticles 345b may achieve relithiation, metal restoration, and doping of microparticles 345c. Upcycled cathode material 365c may be produced by subjecting calcined particles 355c to an additional calcination process (e.g., using calcination component 150 of FIG. 1 ).

[0101] The microparticles 345d may be produced by adding one or more Li precursors, M precursors, P precursors, C precursors, etc. to the second particles 125b to upgrade the morphology, chemical composition, and doping of the second particles 125b (e.g., using the precursor generator 130 and microparticle modification component 140 of FIG. 1 ). The calcined particles 355d may be produced by calcining the microparticles 345d using the calcination component 150 of FIG. 1 . Calcining the microparticles 345d may achieve crystallization, doping, and carbon coating of the microparticles 345d. The upcycled cathode material 365d may be produced by performing surface engineering (e.g., surface coating) on ​​the calcined particles 355d (e.g., using the surface engineering component 160 of FIG. 1 ).

[0102] 4 and 5 are schematic diagrams illustrating exemplary microparticle production reactors 400 and 500 according to some embodiments of the present disclosure.

[0103] As shown in FIG. 4, microparticle production reactor 400 may include droplet generator 410, chamber 420, inlets 431 and 433, powder classification unit 440, and / or any other suitable components for producing microparticles using the spray drying process described herein.

[0104] A precursor solution may be supplied to the chamber 420 via the inlet 431. The droplet generator 410 may include one or more atomizing spray nozzles and / or any other suitable mechanism (e.g., centrifugal droplet generation process) capable of generating fine droplets using the precursor. In the chamber 420, the precursor may be pumped at high pressure through the atomizing spray nozzle. At the outlet of the microdroplet generator, the precursor is aerosolized into fine droplets. Meanwhile, a flow of hot carrier gas may be introduced into the bottom of the chamber 420 via the inlet 433, causing a vortex from the bottom to the top of the chamber 420. The vortex may create a temperature gradient between a high temperature at the bottom of the chamber and a relatively low temperature at the top. The size of the droplets generated by the microparticle generation reactor 400 may be controlled by adjusting spray parameters such as pressure, flow rate, and nozzle geometry. The particles generated in the chamber 420 may be supplied to a powder classification unit 440 for classification. The powder classification unit 440 may include an air classification system or any other suitable system capable of classifying particles by size (e.g., sieve sorting). The powder classification unit 440 may classify the particles produced in the chamber 420 into particles 445a having a desired size and particles 445b lacking the desired size. The particles 445a having the desired size may be collected for further processing. The particles 445b lacking the desired size may be recycled and reused as precursor feedstock.

[0105] Referring to FIG. 5, microparticle production reactor 500 may include droplet generator 510, chamber 520, inlets 531 and 533, powder classification unit 540, one or more filters 550, exhaust system 560, and / or any other suitable components for producing microparticles utilizing the spray granulation process described herein.

[0106] A precursor solution (e.g., a solution or suspension containing solids) may be atomized to form droplets within the fluidized bed system by droplet generator 510. Droplet generator 510 may include one or more atomizing spray nozzles and / or any other suitable mechanism (e.g., centrifugal droplet generation) capable of generating finely divided droplets using the precursor. Meanwhile, a flow of hot carrier gas may be introduced into the bottom of chamber 520 via inlet 533 to induce a vortex from the bottom of chamber 520 to the top of chamber 520 .

[0107] Rapid heat exchange between the hot gas phase and the atomized droplets can result in rapid liquid evaporation and the formation of an initial core of nanoparticles and / or microparticles. As additional droplets are introduced into the system, they come into contact with the initial core. As the surrounding liquid evaporates, the core grows in size, forming even larger particles. This procedure is carried out continuously in the fluidized bed, allowing the granules to grow layer by layer. This layer-by-layer accumulation can produce high-density particles.

[0108] The particles generated in chamber 520 may be fed to powder classification unit 540 for classification. Powder classification unit 540 may include an airflow classification system or any other suitable system capable of classifying particles by size (e.g., sieve sorting). Powder classification unit 540 may classify the particles generated in chamber 520 into particles having a desired size and particles lacking the desired size. Filter 550 may include a filtration system capable of physically separating solid particles from a solid / gas mixture. Exhaust system 560 may direct reaction exhaust gases from the controlled reaction. Particles 543 having the desired size may be collected for further processing. Particles 541 lacking the desired size may be recycled and reused as precursor feedstock.

[0109] 6 illustrates an exemplary baking system 600 according to some embodiments of the present disclosure. Baking system 600 may include an ebullated bed system 610 and a plasma baking system 620. Ebullated bed system 610 may include a chamber 613, a filter 614, and an exhaust system 615. Plasma baking system 620 may include a power source 622, a water-cooled wall 623, a quench zone 624, and a laminar flow zone 625.

[0110] The power source 622 may be any suitable electrical device capable of powering an electrical load in a plasma reaction. The power source may convert current from a power source to the correct voltage, current, and frequency to power the load. The water wall 623 and quench zone 624 act as cooling sections to protect the firing system 600 from high temperatures. The laminar flow zone 625 may allow for a type of fluid flow in which the gas / solid fluid moves in a smooth or regular path.

[0111] A precursor 611 containing cathode material microparticles (e.g., first precursor solution 135a and / or microparticles 145 in Figure 1) may be fed into an ebullated bed system 610. In the ebullated bed, a hot gas stream 612 may enter the ebullated bed chamber 613 from the bottom of the chamber. The hot gas stream can cause decomposition of the precursor compounds within the particles into oxides or phosphates, which can form strong bonds that bind small nanoparticles together within the particles and prevent agglomeration due to incomplete decomposition of the precursor. The decomposition temperature and residence time of the particles within the ebullated bed chamber provide control over the particle porosity and morphology. A continuous air flow can direct the pre-calcined microparticles 621 into a warm plasma reactor. An internal plasma discharge can briefly raise the particle temperature to 1500-2000°C, forming molten microdroplets. The plasma temperature and temperature profile along the particle flow path within this in-line plasma calcination zone are controlled by various parameters to achieve a final, well-calcined material. The relatively high surface area of ​​the entrained powder allows for complete firing in a much shorter time compared to bulk firing in a static furnace.

[0112] After in situ plasma calcination, two channels exist for the calcined particles. In the first channel, the calcined particles 626 may be collected for post-treatment. In the second channel, the hot gas and powder exit through the bottom of the heating zone and may be entrained in the high-flow region of the system. The flow rate of the carrier gas entrained in the high-flow region of the system is much higher than the flow rate through the spray-drying chamber, causing a sudden drop in particle temperature as heat is dissipated to the much larger volume of gas. Via this high-velocity gas flow, the calcined particles are transported to the surface engineering reactor described herein.

[0113] 7 shows an exemplary surface engineering reactor 700 according to some embodiments of the present disclosure. The surface engineering reactor 700 may include a spray coating system 710 and an ebullated bed system 750. The spray coating system 710 may include a droplet generator 713, a chamber 715, a filter 717, and an exhaust system 719. The ebullated bed system 750 may include an ebullated bed 753, a powder collector 755, and an exhaust system 757.

[0114] The droplet generator 705 may include one or more nozzles and / or any other suitable mechanism for generating a spray of the coating precursor 701. The calcined particles produced by the calcination system 600 may be coated with the precursor in the chamber 715. A hot gas stream of carrier gas 703 may be introduced into the chamber 715 through the bottom of the chamber 715. The precursor solution sprayed into the chamber 715 may cause turbulence and thorough mixing of the particles, resulting in a uniform coating on the surface of the calcined particles. The carrier gas, separated from the previously entrained powder, may exit the chamber 715 and enter the exhaust system 719 directly. After the particles are coated with the precursor, the coated particles may be transported to the ebullated bed 753 (also referred to as the second ebullated bed). The hot gas stream 707 may enter the ebullated bed system 750 from the bottom of the chamber 751 and cause the decomposition of the coating precursor on the particles into oxides to form a uniform surface coating. The coated particles may be collected in the powder collector 755.

[0115] Spray coating in the surface engineering reactor 700 can produce an optimal surface coating on the calcined particles. When coating using a solution or suspension, the liquid helps transport the solids to the surface of the particles. The coating techniques described herein can allow for optimal retention time of the particles in the surface engineering reactor 700, thereby ensuring excellent coating quality.

[0116] 8A is a flowchart of an exemplary process 800 for upcycling spent batteries according to some embodiments of the present disclosure. Process 800 may be implemented using system 100 of FIG. 1, microparticle production reactor 400 of FIG. 4, microparticle production reactor 500 of FIG. 5, calcination system 600 of FIG. 6, and / or surface engineering reactor 700 of FIG. 7.

[0117] At 810, the cathode material of the spent battery may be separated into a plurality of particle groups of various sizes and / or shapes. For example, a first particle group may include first particles of a first size, and a second particle group may include second particles of a second size. The first particles and second particles may be first particles 125a and second particles 125b, as described in connection with FIG. 1 above. The cathode material may be separated by a particle separator 120, as described in connection with FIG. 1 above.

[0118] At 820, a first precursor solution may be generated using the first group of particles. The first precursor solution may include at least one of a suspension containing the first group of particles or a solution containing the first group of particles. In some embodiments, the first precursor solution may include at least one of LiOH, LiNO, LiAc, Ni(NO), Mn(NO), Co(NO), CHONi, Ni(Ac), CHOMn, Mn(Ac), C 12 H 10 MnO 14 , C2H2O4Co, Co(Ac)2, or Al(NO3)3. In some embodiments, the first precursor solution may include a lithium precursor and a doping precursor. In some embodiments, the dopant precursor may include one or more of an Al dopant precursor, a Mg dopant precursor, a Ti dopant precursor, a Ca dopant precursor, a Nb dopant precursor, a Zr dopant precursor, a W dopant precursor, a Te dopant precursor, an F dopant precursor, or a Mo dopant precursor. The first precursor solution may be generated by a precursor generator 130, as described in connection with FIG. 1 above.

[0119] At 830, a second precursor solution may be generated using the second set of particles. The second precursor solution may include at least one of a suspension containing the first set of particles or a solution containing the first set of particles. In some embodiments, the second precursor solution may include at least one of LiOH, LiNO, LiAc, Ni(NO), Mn(NO), Co(NO), CHONi, Ni(Ac), CHOMn, Mn(Ac), C12 H 10 MnO 14 , C2H2O4Co, Co(Ac)2, Al(NO3)3, or a dopant precursor. In some embodiments, the second precursor solution may include one or more of a Li precursor, a Mn precursor, a Co precursor, an Al precursor, etc. In some embodiments, the second precursor solution may include one or more of an Al dopant precursor, a Ti dopant precursor, a Mg dopant precursor, a Ca dopant precursor, a Nb dopant precursor, a Zr dopant precursor, a W dopant precursor, a Te dopant precursor, an F dopant precursor, or a Mo dopant precursor. The second precursor solution may be generated by a precursor generator 130, as described in connection with FIG. 1 above.

[0120] At 840, a first cathode material may be produced using the first precursor solution. For example, as shown in FIG. 8B, at 841, the first precursor solution may be calcined to produce first calcined particles. Calcining the first precursor solution may relithiate and dope the first particles. More specifically, for example, calcination component 150 may produce first calcined particles 155a using first precursor solution 135a, as described in connection with FIGS. 1-2 above.

[0121] At 843, the first fired particles may be surface engineered. For example, a spray coating process may be performed by surface engineering component 160, as described above in connection with Figures 1 and 7. The first cathode material may be first cathode material 165a, as described above in connection with Figures 1 and 2.

[0122] At 850, a second cathode material may be produced using the second precursor solution. For example, as shown in FIG. 8C, at 851, a plurality of microparticles may be formed using the second precursor solution. More specifically, for example, the microparticle-modifying component 140 may produce microparticles 145 using the second precursor solution 135b, as described in connection with FIG. 1 above. The microparticles may include one or more calcined particles 355a, 355b, 355c, and 355d, as described in connection with FIG. 3B.

[0123] In 853, the plurality of microparticles may be calcined to produce second calcined particles. More specifically, for example, the calcination component 150 may use the second precursor solution 135b to produce second calcined particles 155b, as described above in connection with FIGS. 1-3.

[0124] The second fired particles may be surface engineered at 855. The second cathode material may be and / or include the second cathode material 165b of FIG. 1 and the upcycled cathode materials 365a, 365b, 365c, 365d of FIG. 3B.

[0125] Figure 9A shows an SEM image of aged NCA lithium-ion cathode material, in which severe particle cracking can be observed. Figure 9C shows morphology-modified NCA lithium-ion battery cathode material particles derived from the fractured nanoparticles shown in Figure 9B, achieved under optimized conditions. These secondary particles maintain a uniform spherical morphology with a densely packed structure. Within these particles, primary particles are uniformly distributed across their cross-section, highlighting their dense nature. Particle size analysis reveals that 50% of these particles have diameters less than 13 μm. The creation of these microscale spherical secondary particles can significantly increase tap density, proving beneficial for electrode fabrication. The electrochemical performance of the developed NCA cathode material was evaluated using a half-cell coin cell. As shown in Figure 9D, the modified NCA cathode material exhibits cycling performance comparable to that of the commercial NCA sample.

[0126] In contrast to polycrystalline particles, layered NCM materials made from single-crystalline particles and lacking grain boundaries reduce interparticle stress during high charge states and are less susceptible to particle fracture. Furthermore, single-crystalline NCM particles are more resistant to detrimental electrolyte attack. Figure 10B shows an SEM image of single-crystalline NCM622 regenerated from damaged NCM111 polycrystalline particles using a specific annealing process. The XRD pattern shown in Figure 10A verifies the crystalline phase of the layered single-crystalline NCM622. Half cells were assembled using a commercial polycrystalline NCM622 (PS-NCM622) cathode and a regenerated single-crystalline NCM622 (SC-NCM622) cathode. As shown in Figures 10C and 10D, the regenerated SC-NCM622 is slightly superior to the commercial PS-NCM622 in aspects such as initial discharge specific capacity, first coulombic efficiency, and cyclability.

[0127] Figure 11A shows the aged and purified LFP cathode material containing nanoparticles. Figure 11B shows spray-dried LiFePCL microparticles post-annealed at 700 °C for 5 h in an argon atmosphere using a carefully selected precursor suspension (containing spent LFP nanoparticles, a lithium source, a solvent, and a binder). Both particles maintain a spherical morphology with a D50 equivalent to 9.7 μm, as shown in Figure 11C. Figure 11D shows the specific discharge capacity and cyclability of the pristine LFP nanoparticle cathode material (vs. Li / Li+) compared with the regenerated LFP microparticle cathode material in a C / 5 half cell. Figure 11D shows that the regenerated LFP cathode material achieves a significantly higher discharge capacity (150 mAh / g) than the pristine LFP cathode (134 mAh / g), indicating complete recovery of lithium ions within the spent LFP crystal structure.

[0128] For LMFP regeneration, in addition to lithium, LiMn 0.5 Fe 0.5 Additional Mn and P sources are essential to maintain the chemical balance toward PO4. Similar to the regenerated LFP microparticles, the regenerated LMFP adopts a spherical morphology, as shown in Figure 12A. As shown in Figure 12B, the primary particles are densely packed and agglomerated, with minimal void space, while the secondary particles are highly spherical, with an average diameter of 9.67 μm (D50). XRD characterization of the regenerated LFP microparticles and the regenerated LMFP microparticles is shown in Figure 12C. Both samples closely match the diffraction patterns of LiMnPO4 and LiFePO4, both of which belong to the Pmnb(62) space group. Notably, no impurity phases were detected, highlighting the high purity of the regenerated products. The electrochemical performance of the regenerated LFP and LMFP cathode materials is shown in Figure 12D. While both samples offer similar discharge capacities of approximately 150 mAh / g, the recycled LMFP cathode exhibits improved energy density compared to LFP, shifting from 500 Wh / kg to 600 Wh / kg, representing an improvement of approximately 20% due to the increased operating voltage.

[0129] For ease of explanation, the methods of the present disclosure are depicted and described as a series of acts. However, acts according to the present disclosure may occur in various orders and / or simultaneously, and with other acts not shown and described herein. Moreover, not all illustrated acts may be required to implement a methodology in accordance with the disclosed subject matter. In addition, those skilled in the art will understand and appreciate that a methodology could alternatively be represented as a series of interrelated states via a state diagram or events.

[0130] The terms "approximately," "about," and "substantially" can be used to mean, in some embodiments, within ±20% of a target dimension, in some embodiments, within ±10% of a target dimension, in some embodiments, within ±5% of a target dimension, and even in some embodiments, within ±2% of a target dimension. The terms "approximately" and "about" can be inclusive of the target dimension.

[0131] Although the foregoing description sets forth numerous details, it will be apparent that the present disclosure may be practiced without these specific details. In some instances, well-known structures and devices are shown in block diagram form, rather than in detail, in order to avoid obscuring the present disclosure.

[0132] As used herein, the terms "first," "second," "third," "fourth," etc., refer to labels for distinguishing different elements and do not necessarily imply an order according to their numerical designation.

[0133] The words "example" or "exemplary" are used herein to mean serving as an example, instance, or illustration. Any aspect or design described herein as "example" or "exemplary" should not necessarily be construed as preferred or advantageous over other aspects or designs. Rather, use of the words "example" or "exemplary" is intended to present a concept in a concrete manner. As used in this application, the term "or" is intended to mean an inclusive "or" rather than an exclusive "or." That is, unless otherwise specified or clear from the context, "X includes A or B" is intended to mean any of the natural inclusive permutations. That is, if X includes A, or X includes B, or X includes both A and B, then "X includes A or B" is satisfied under any of the foregoing cases. Additionally, the articles "a" and "an," as used in this application and the appended claims, should generally be construed to mean "one or more" unless otherwise specified or clear from the context that the singular form is intended. References throughout this specification to an "implementation" or "one implementation" mean that a particular feature, structure, or characteristic described in connection with that implementation is included in at least one implementation. Thus, appearances of the phrase "implementation" or "one implementation" in various places throughout this specification are not necessarily all referring to the same implementation.

[0134] Although many variations and modifications of the present disclosure will become apparent to those skilled in the art after reading the foregoing description, it should be understood that any particular embodiments shown and described by way of illustration are in no way intended to be considered limiting. Accordingly, references to details of various embodiments are not intended to limit the scope of the claims, which themselves recite only those features that are deemed to be part of the present disclosure.

Claims

1. 1. A method for upcycling used batteries, comprising: separating the cathode material of the spent battery into a plurality of particle groups; Including, a first group of the plurality of particle groups comprising first particles of a first size, and a second group of the plurality of particle groups comprising second particles of a second size; The method further comprises: generating a first precursor solution using the first particles; generating a second precursor solution using the second particles; producing a first cathode material using the first precursor solution; producing a second cathode material using the second precursor solution; A method comprising:

2. The method of claim 1 , wherein the first particle is a microparticle and the second particle is a nanoparticle.

3. The method of claim 1 , wherein the first precursor solution comprises at least one of a suspension containing the first particles and a solution containing the first particles.

4. The first precursor solution is LiOH, LiNO ３ , LiAc, Ni(NO ３ ) ２ , Mn(NO ３ ) ２ , Co(NO ３ ) ２ , C ２ H ２ O ４ Ni, Ni(Ac) ２ , C ２ H ２ O ４ Mn, Mn(Ac) ２ , C １２ H １０ Mn ３ O １４ , C ２ H ２ O ４ Co, Co(Ac) ２ and Al(NO ３ ) ３ The method of claim 3 , further comprising at least one of:

5. 4. The method of claim 3, wherein the first precursor solution comprises one or more dopant precursors, the one or more dopant precursors comprising at least one of Al, Ti, Mg, Ca, Nb, Zr, W, Te, Mo, and F.

6. The method of claim 3 , wherein the first precursor solution further comprises a lithium precursor.

7. producing the first cathode material using the first precursor solution, calcining the first precursor solution to form first calcined particles; performing surface engineering on the first calcined particles; The method of claim 1 , comprising:

8. producing the second cathode material using the second precursor solution; forming a plurality of microparticles using the second precursor solution; calcining the plurality of microparticles to form second calcined particles; The method of claim 1 , comprising:

9. 10. The method of claim 8, wherein forming the plurality of microparticles using the second precursor solution comprises utilizing at least one of a spray granulation process or a spray drying process to produce micronized droplets.

10. 10. The method of claim 9, wherein producing the second cathode material using the second precursor solution further comprises performing surface engineering on the second calcined particles.

11. The method of claim 1 , wherein the second precursor solution comprises at least one of a suspension containing the second particles and a solution containing the second particles.

12. The second precursor solution is LiOH, LiNO ３ , LiAc, Ni(NO ３ ) ２ , Mn(NO ３ ) ２ , Co(NO ３ ) ２ , C ２ H ２ O ４ Ni, Ni(Ac) ２ , C ２ H ２ O ４ Mn, Mn(Ac) ２ , C １２ H １０ Mn ３ O １４ , C ２ H ２ O ４ Co, Co(Ac) ２ and Al(NO ３ ) ３ The method of claim 11 , comprising at least one of:

13. The second precursor solution contains a Li precursor, and the Li precursor is LiOH, LiNO ３ and LiAc.

14. The second precursor solution includes a Mn precursor, and the Mn precursor is Mn(Ac). ２ , Mn(NO ３ ) ２ , C ２ H ２ O ４ Mn, C １２ H １０ Mn ３ O １４ and Mn(NO ２ ) ２ The method of claim 12 , comprising at least one of:

15. The second precursor solution includes a Co precursor, and the Co precursor is Co(Ac). ２ , Co(NO ３ ) ２ , C ２ H ２ O ４ Co and Co(NO ２ ) ２ The method of claim 12 , comprising at least one of:

16. The second precursor solution includes an Al precursor, and the Al precursor is Al[OCH(CH ３ ) ２ ] ３ , Al(N(CH ３ ) ２ ) ３ , Al[OCH(CH ３ ) C ２ H ５ ] ３ , (CH ３ ) ３ Al and Al(NO ３ ) ３ The method of claim 12 , comprising at least one of:

17. 13. The method of claim 12, wherein the second precursor solution comprises one or more dopant precursors, the one or more dopant precursors comprising at least one of Al, Ti, Mg, Ca, Nb, Zr, W, Te, Mo, and F.

18. a particle separator configured to separate the cathode material of the spent battery into a plurality of particle populations, a first population of the plurality of particle populations including first particles of a first size and a second population of the plurality of particle populations including second particles of a second size; forming a first precursor solution using the first particles; generating a second precursor solution using the second particles; a precursor generator configured as follows: forming a first cathode material using the first precursor solution; using the second precursor solution to form a second cathode material; a battery upgrade component configured to A system comprising:

19. 20. The system of claim 18, wherein the first particle is a microparticle and the second particle is a nanoparticle.

20. the battery upgrade component comprises: a microparticle-modifying component configured to form a plurality of microparticles using the second precursor solution; calcining the first precursor solution to form first calcined particles; calcining the plurality of microparticles to form second calcined particles; A firing component configured as follows: a surface engineering component configured to perform surface engineering on the first calcined particles; 20. The system of claim 18, further comprising:

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