AU2021324137A1

AU2021324137A1 - Process for recovering values from batteries

Info

Publication number: AU2021324137A1
Application number: AU2021324137A
Authority: AU
Inventors: Andrew Mackenzie; Andrew NAPIER; Andrew SKALSKI
Original assignee: Resource Conservation And Recycling Corp Pty Ltd
Current assignee: Resource Conservation And Recycling Corp Pty Ltd
Priority date: 2020-08-12
Filing date: 2021-08-12
Publication date: 2023-03-30
Also published as: WO2022032345A1

Abstract

The present disclosure relates generally to processes for recovering values from batteries. More specifically, the present disclosure relates to processes for recovering an electrode material from lithium-ion batteries, such as an electrode material comprising a cathode material and/or an anode material, for example a mixed metal material (MMD).

Description

PROCESS FOR RECOVERING VALUES FROM BATTERIES

TECHNICAL FIELD

[0001] The present disclosure relates generally to processes for recovering values from batteries. More specifically, the present disclosure relates to processes for recovering an electrode material from lithium-ion batteries, such as an electrode material comprising a cathode material and/or an anode material, for example a mixed metal material (MMD).

BACKGROUND

[0002] Lithium-ion batteries are increasingly being used to power automotive, consumer, electronic, and industrial energy storage applications. For example, lithium- ion batteries are used in personal devices (laptops, and smart phones etc.), power tools, bicycles, power storage and light and heavy vehicles, such as trams and trains.

[0003] As lithium-ion batteries reach their end-of-life, it is often desirable to recycle and dispose of them whilst recovering one or more values for on-sale and/or re-use. Current lithium-ion battery recycling often requires smelting or pyrometallurgical processing to extract one or more values. However, such processes often extract values as complex alloys with steel while additional valuable components are trapped as part of the slag phase and/or decomposed at the high temperature. As such, further processing of the slag material/alloys to obtain values requires high cost and additional processing steps.

[0004] Other recycling process include physically shredding the lithium-ion batteries into smaller components. However, such shredding processes can also generate high temperatures and is often mitigated via battery pre-treatment (e.g. freezing) and/or shredding in a dry inert atmosphere, requiring specialist process equipment and expensive reagents. [0005] Accordingly, there is a need for recycling process which overcomes one or more of these disadvantages and/or provides the public with a useful alternative.

SUMMARY

[0006] The present inventors have undertaken research and development into processes for recovering one or more values from lithium-ion batteries. In particular, the inventors have identified that subjecting the lithium-ion batteries to shredding in a wet environment (e.g. in the presence of an aqueous stream) can result in the selective separation of values based on the size of particles generated during the shredding step. Additionally, in some embodiments, the present inventors have identified that the aqueous stream can also be used to mitigate the high temperatures generated during conventional dry shredding, while also mitigating one or more halide by-products (e.g. hydrofluoric acid (HF)) that can be generated by the liberation of the electrolyte compounds during the shredding of the lithium-ion batteries and/or be processed to recover/remove one or more values derived from the battery electrolyte, such as lithium, phosphate and fluorine. The present disclosure described herein can also be scalable for industrial application, and finds use in the recovery of values from batteries, such as a mixed metal material (MMD) obtained from lithium-ion batteries.

[0007] A variety of values can be recovered from lithium-ion batteries using the process described herein. In one particular embodiment, the process described herein can obtain an electrode material from lithium-ion batteries. The process comprises shredding lithium-ion batteries in the presence of an aqueous stream. The aqueous stream may be a continuous aqueous input stream. The shredding of the batteries in the presence of the aqueous stream generates a first aqueous slurry stream comprising shredded batteries. The shredded batteries may be in the form of shredded battery particles. At least some of the shredded battery particles comprise the electrode material. The shredded battery particles may also vary in size (e.g. comprise at least a coarse fraction and a fine fraction) . The first aqueous slurry stream also comprises an electrolyte. The electrolyte is liberated from the battery during the shredding process. The electrolyte may be dissolved or suspended in the aqueous phase of the first aqueous slurry stream.

[0008] The shredded battery particles comprising the electrode material may be separated from the first aqueous slurry stream thereby recovering the electrode material resulting in one or more aqueous liquid streams comprising dissolved or suspended electrolyte being produced. In some embodiments, at least part of one or more of the aqueous liquid streams comprising the dissolved or suspended electrolyte may either be recycled back to the shredding step for use in the aqueous input stream, for example as part of a continuous aqueous input stream. Alternatively or additionally, at least part of one or more of the aqueous liquid streams comprising the dissolved or suspended electrolyte may be further treated to remove one or more inorganic and organic species present in the first aqueous liquid stream, for example fluorine, phosphate and/or lithium. In some embodiments, the process may generate multiple aqueous liquid streams, for example a first aqueous liquid stream and second aqueous liquid stream, both comprising dissolved or suspended electrolyte. In some embodiments, at least part of one aqueous liquid stream generated during the process is recycled back to the shredding step for use in the aqueous input stream.

[0009] In some embodiments, at least part of an aqueous liquid stream comprising the dissolved or suspended electrolyte may be recycled to the shredding step for use in the aqueous input stream. At least according to some examples or embodiments described herein, the recycling of at least part of an aqueous liquid stream comprising the dissolved or suspended electrolyte can maintain a more alkaline pH (e.g. a more basic pH) of the aqueous input stream which advantageously can mitigate and/or neutralise one or more halide by-products (e.g. hydrofluoric acid (HF)) which can be generated by the liberation of the electrolyte compounds during the shredding of the lithium-ion batteries. Such by-products can corrode processing equipment/materials.

[0010] At least according to some examples or embodiments described herein, the recycling of at least part of an aqueous liquid stream comprising the dissolved or suspended electrolyte may also avoiding the need for adding external hazardous and/or expensive alkali reagents (e.g. lime) to increase the pH of the aqueous stream thus reducing cost and specific process equipment and redundancy required for the addition of additional strong alkali reagents.

[0011] In one aspect, there is provided process for obtaining an electrode material from lithium-ion batteries, the process comprising the steps of: a) shredding lithium-ion batteries in the presence of a continuous aqueous input stream to obtain a first aqueous slurry stream comprising an aqueous phase, shredded battery particles and an electrolyte, wherein the particles comprise coarser particles of copper, aluminium, plastic and steel and finer particles of electrode material, and the electrolyte is dissolved or suspended in the aqueous phase of the first aqueous slurry stream; b) separating and obtaining the coarser particles of copper, aluminium, plastic and steel and finer particles of electrode material from the first aqueous slurry stream and producing a first aqueous liquid stream comprising dissolved or suspended electrolyte; and c) recycling at least part of the first aqueous liquid stream comprising dissolved or suspended electrolyte to the shredding at step a) for use in the continuous aqueous input stream.

[0012] In some embodiments, step b) further comprises the separating and obtaining of the coarser and finer particles from the first aqueous slurry stream and producing a first aqueous liquid stream and a second aqueous liquid stream, wherein the first and second aqueous liquid streams each comprise dissolved or suspended electrolyte.

[0013] In some embodiments, the separating and obtaining of the coarser and finer particles at step b) comprises separating and obtaining the coarser particles of copper, aluminium, plastic and steel from the first aqueous slurry stream to obtain a separated first aqueous slurry stream comprising the finer particles of electrode material, and separating and obtaining the finer particles of electrode material from the separated first aqueous slurry stream and producing the first aqueous liquid stream. [0014] In some embodiments, separating and obtaining the particles at step b) comprises: bl) dewatering and classifying the first aqueous slurry stream comprising the shredded battery particles based on particle size to produce a second aqueous slurry stream comprising the coarser particles, a third aqueous slurry stream comprising the finer particles, and the first aqueous liquid stream; b2) subjecting the second aqueous slurry stream comprising the coarser particles to further shredding to obtain a sized reduced second aqueous slurry stream; and b3) combining the size-reduced second aqueous slurry stream with the third aqueous slurry stream to obtain the first aqueous slurry stream and separating the particles therefrom and producing a second aqueous liquid stream comprising dissolved or suspended electrolyte and optionally recycling at least part of the second aqueous liquid stream comprising dissolved or suspended electrolyte to the shredding at step a) for use in the continuous aqueous input stream.

[0015] In some embodiments, at least part of the second aqueous liquid stream comprising dissolved or suspended electrolyte is optionally recycled to the shredding at step a) for use in the continuous aqueous input stream.

[0016] In some embodiments, the recycling of the first aqueous liquid stream comprising the dissolved or suspended electrolyte is provided to maintain the pH of the continuous aqueous input stream between about pH 6 to about pH 12, about pH 7 to about 11, or about pH 8 to about pH 10. By maintaining the continuous aqueous input stream having a more alkaline pH (e.g. less acidic pH), the generation of one or more halide by-products (e.g. hydrofluoric acid (HF)) can be mitigated. In one embodiment, the continuous aqueous input stream does not comprise lime.

[0017] In some embodiments, the continuous aqueous input stream has a flow rate of between about 0.1 m³/tonne to about 100 m³/tonne, or about 30 m³/tonne to about 50 m³/tonne of aqueous input per tonne of lithium-ion battery. By controlling the continuous flow rate of the aqueous input stream, further advantages can be provided according to at least some examples or embodiments described herein, including mitigating fire and dust generation, and/or avoiding the need to submerge the shredding, classification and dewatering equipment in water, simplifying the design, safety and operation of this equipment.

[0018] In some embodiments, the first aqueous slurry stream is subjected to further shredding to reduce the average particle size of the shredded battery particles prior to separating the particles at step b). In some embodiments, the further shredding is performed in the absence of a continuous aqueous input stream, which according to at least some examples and embodiments described herein, provides a shredded product of the appropriate size that can be separated in step b) without the requirement for further processing steps, such as dewatering.

[0019] In some embodiments, the first aqueous slurry stream is subjected to further shredding to reduce the average particle size of the shredded battery particles prior to separating the particles at step b). In some embodiments, the further shredding is performed in the presence of a continuous aqueous input stream, which according embodiments described herein, provides a shredded product of the appropriate size that can be separated in step b).

[0020] In some embodiments, the process further comprises washing and/or attritioning the first aqueous slurry stream comprising the coarser particles of copper, aluminium, plastic and steel and finer particles of electrode material prior to step b). By washing and/or attritioning the shredded battery particles in the presence of the coarser particles (such as the magnetic steel particles), further advantages can be provided according to at least some examples or embodiments described herein, including improved liberation and recovery of electrode materials without the use of toxic stripping solvents. In some embodiments, the first aqueous slurry stream is not stripped with a stripping solvent prior to separating the particles therefrom at step b).

[0021] In some embodiments, the first and/or second aqueous liquid stream comprising dissolved or suspended electrolyte may be further treated to remove one or more inorganic and organic species (e.g. electrolyte values) present in the aqueous liquid stream. In some embodiments, the first and/or second aqueous liquid streams comprising dissolved or suspended electrolyte are combined prior to further treatment to remove one or more inorganic and inorganic species.

[0022] It will be appreciated that other aspects, embodiments and examples of the processes and materials are described herein.

BRIEF DESCRIPTION OF FIGURES

[0023] Notwithstanding any other forms which may fall within the scope of the process described herein, specific embodiments will now be described, by way of example only, with reference to the accompanying figures in which:

[0024] Figure 1: Process flow sheet depicting a process for obtaining an electrode material from lithium-ion batteries.

[0025] Figure 2: Process flow sheet depicting a process for obtaining an electrode material from lithium-ion batteries and one or more other values liberated from the battery during shredding.

[0026] Figures 3 and 4: Process flow sheet depicting a process for obtaining an electrode material from lithium-ion batteries, incorporating either a wet or dry copper, aluminium and plastic separation.

[0027] Figure 5: Process flow sheet depicting a process for obtaining an electrode material from lithium-ion batteries, incorporating gravity separation of the electrode material to separate cathode and anode material. DETAILED DESCRIPTION

[0028] The present disclosure describes the following various non-limiting embodiments, which relates to investigations undertaken to identify processes for recovering one or more values from lithium-ion batteries.

General terms

[0029] In the following description, reference is made to the accompanying drawings which form a part hereof, and which is shown, by way of illustration, several embodiments. It is understood that other embodiments may be utilized and structural changes may be made without departing from the scope of the present disclosure.

[0030] With regards to the definitions provided herein, unless stated otherwise, or implicit from context, the defined terms and phrases include the provided meanings. Unless explicitly stated otherwise, or apparent from context, the terms and phrases below do not exclude the meaning that the term or phrase has acquired by a person skilled in the relevant art. The definitions are provided to aid in describing particular embodiments, and are not intended to limit the claimed invention, because the scope of the invention is limited only by the claims. Furthermore, unless otherwise required by context, singular terms shall include pluralities and plural terms shall include the singular.

[0031] All publications discussed and/or referenced herein are incorporated herein in their entirety.

[0032] Any discussion of documents, acts, materials, devices, articles or the like which has been included in the present specification is solely for the purpose of providing a context for the present disclosure. It is not to be taken as an admission that any or all of these matters form part of the prior art base or were common general knowledge in the field relevant to the present disclosure as it existed before the priority date of each claim of this application. [0033] Throughout this disclosure, unless specifically stated otherwise or the context requires otherwise, reference to a single step, composition of matter, group of steps or group of compositions of matter shall be taken to encompass one and a plurality (i.e., one or more) of those steps, compositions of matter, groups of steps or groups of compositions of matter. Thus, as used herein, the singular forms “a”, “an” and “the” include plural aspects unless the context clearly dictates otherwise. For example, reference to “a” includes a single as well as two or more; reference to “an” includes a single as well as two or more; reference to “the” includes a single as well as two or more and so forth.

[0034] Those skilled in the art will appreciate that the disclosure herein is susceptible to variations and modifications other than those specifically described. It is to be understood that the disclosure includes all such variations and modifications. The disclosure also includes all of the examples, steps, features, methods, compositions, coatings, processes, and coated substrates, referred to or indicated in this specification, individually or collectively, and any and all combinations or any two or more of said steps or features.

[0035] Unless otherwise defined, all technical and scientific terms used herein have the same meaning commonly understood by one of ordinary skill in the art to which this invention belongs. Although methods and materials similar or equivalent to those described herein can be used in the practice or testing of the present invention, suitable methods and materials are described below. In case of conflict, the present specification, including definitions, will control. In addition, the materials, methods, and examples are illustrative only and not intended to be limiting.

[0036] The term “and/or”, e.g., “X and/or Y” shall be understood to mean either “X and Y” or “X or Y” and shall be taken to provide explicit support for both meanings or for either meaning.

[0037] Unless otherwise indicated, the terms “first,” “second,” etc. are used herein merely as labels, and are not intended to impose ordinal, positional, or hierarchical requirements on the items to which these terms refer. Moreover, reference to a “second” item does not require or preclude the existence of lower-numbered item (e.g., a “first” item) and/or a higher-numbered item (e.g., a “third” item).

[0038] As used herein, the phrase “at least one of’, when used with a list of items, means different combinations of one or more of the listed items may be used and only one of the items in the list may be needed. The item may be a particular object, thing, or category. In other words, “at least one of’ means any combination of items or number of items may be used from the list, but not all of the items in the list may be required. For example, “at least one of item A, item B, and item C” may mean item A; item A and item B; item B; item A, item B, and item C; or item B and item C. In some cases, “at least one of item A, item B, and item C” may mean, for example and without limitation, two of item A, one of item B, and ten of item C; four of item B and seven of item C; or some other suitable combination.

[0039] As used herein, the term “about”, unless stated to the contrary, typically refers to +/- 10%, for example +/- 5%, of the designated value.

[0040] It is to be appreciated that certain features that are, for clarity, described herein in the context of separate embodiments, may also be provided in combination in a single embodiment. Conversely, various features that are, for brevity, described in the context of a single embodiment, may also be provided separately or in any subcombination.

[0041] Throughout the present specification, various aspects and components of the invention can be presented in a range format. The range format is included for convenience and should not be interpreted as an inflexible limitation on the scope of the invention. Accordingly, the description of a range should be considered to have specifically disclosed all the possible sub-ranges as well as individual numerical values within that range, unless specifically indicated. For example, description of a range such as from 1 to 5 should be considered to have specifically disclosed sub-ranges such as from 1 to 3, from 1 to 4, from 1 to 5, from 2 to 4, from 2 to 5, from 3 to 5 etc., as well as individual and partial numbers within the recited range, for example, 1, 2, 3, 4, 5, 5.5 and 6, unless where integers are required or implicit from context. This applies regardless of the breadth of the disclosed range. Where specific values are required, these will be indicated in the specification.

[0042] Throughout this specification the word "comprise", or variations such as "comprises" or "comprising", will be understood to imply the inclusion of a stated element, integer or step, or group of elements, integers or steps, but not the exclusion of any other element, integer or step, or group of elements, integers or steps.

[0043] Each example of the present disclosure described herein is to be applied mutatis mutandis to each and every other example unless specifically stated otherwise. The present disclosure is not to be limited in scope by the specific examples described herein, which are intended for the purpose of exemplification only. Functionally equivalent products, compositions and methods are clearly within the scope of the disclosure as described herein.

Specific terms

[0044] As used herein, the term “electrode material” refers to a material comprising either anode material, cathode material or a mixture thereof. In the context of the present disclosure, the electrode material is obtained from lithium-ion batteries, and comprise or consist of a mixed metal material.

[0045] As used herein, the term “mixed metal material” includes any compound comprising at least two metals. By way of example, where the mixed metal material is obtained during the recycling of lithium-ion batteries, the mixed metal material may comprise one or more metals that are present in lithium-ion batteries, such as those present in the electrodes (e.g. cathode and anode materials). As an example, the metals in the mixed metal material may comprise nickel and cobalt metal values. Other nonlimiting examples of metals in the mixed metal material can include aluminium, carbon, cobalt, copper, iron, lithium, magnesium, manganese, nickel, phosphorous, titanium and zinc. The mixed metal material may be a mixed metal dust (MMD) (also referred to as a mixed metal oxide dust and “black mass”). In some embodiments, the MMD may be obtained during the recycling of lithium-ion batteries. The MMD may be a blend of one or more cathode and anode materials obtained from lithium-ion batteries. In some embodiments, the MMD comprises lithium nickel manganese cobalt oxide (NMC), lithium cobalt oxide (LCO) or lithium nickel cobalt aluminium oxide (NCA), lithium manganese oxide (LMO), lithium ferro phosphate (LFP), lithium titanate (LTO) or a mixture thereof. The mixed metal material may comprise a plurality of particles.

[0046] As used herein, the term “precipitate” or “precipitation” refers to the formation of an insoluble solid from a solution. The precipitate may form as a result of a chemical reaction (e.g. via the addition of an appropriate precipitant to the solution). Alternatively, a precipitate may form if a material dissolved in a liquor exceeds its solubility limit, such as by changing the liquids temperature. Depending on the nature of the precipitation, the precipitate may be an amorphous precipitate, or comprise one or more crystals e.g. crystalline precipitate. In some embodiments, the precipitation may also induce crystallisation.

[0047] A reference to “g/kg”, “g/g” or “kg/f ’ throughout the specification refers to the mass of a substance per kilogram, gram or tonne, respectively, of the total weight of a composition. A reference to “g/L” throughout the specification refers to the mass of a substance per litre of the total volume of a liquid. A reference to “% w/w” or “% w/v” throughout the specification refers to the percentage amount of a substance in a composition on a weight or volume basis, respectively.

[0048] As used herein, the term “solids concentration” refers to the percentage of solids present in a composition, for example the % of solids present in a slurry stream or liquid stream. This can be calculated by dividing the total weight of solids present in the slurry or liquid stream (for example present in a representative sample or aliquot of the slurry or liquid stream) by the total weight of the slurry or liquid stream (e.g. the mass of the representative sample of aliquot) multiplied by 100. Solids concentration can be provided in the terms of % w/w, as defined above.

[0049] As used herein, reference to the term “slurry” throughout the specification refers to a stream comprising solids and liquids. The solids concentration (in % w/w) of the slurry can vary as described herein. In some embodiments, a slurry described herein may comprise a high % w/w solids concentration (e.g. greater than 80% w/w). In some embodiments, a slurry comprising a higher % w/w solids concentration may also be called a solids stream as understood by the skilled person.

Process for recovering values from lithium-ion batteries

[0050] The process described herein can recover one or more values from lithium-ion batteries, namely materials that make up the “electrode material (e.g. cathode and anode materials), electrolyte; and materials from the separator, casing/housing and other auxiliary components.

[0051] The cathode (also known as the positive electrode) comprises a lithium metal oxide which can vary depending on the battery type, application and/or manufacturer. In some embodiments, the cathode material may be lithium nickel manganese cobalt oxide (NMC), lithium cobalt oxide (LCO) or lithium nickel cobalt aluminium oxide (NCA), lithium manganese oxide (LMO), lithium ferro phosphate (LFP), lithium titanate (LTO) and mixtures thereof. In some embodiments, the cathode material may comprise a “mixed metal material” or a “mixed metal oxide” or “MMD” as described above. The anode (also known as the negative electrode) usually comprises graphite.

[0052] The electrolyte promotes the movement of ions from the cathode to the anode on charge and in reverse on discharge. Examples of electrolyte lithium containing compounds, for example, hexafluorophosphate (LiPFe), lithium tetrafluorob orate (LiBF4), lithium perchlorate (LiCICU), lithium hexafluoroarsenate monohydrate (LiAsFe), lithium trifluoromethanesulfonate (LiCFsSCh), lithium bis(bistrifluoromethanesulfonyl)imide (LiTFSI), lithium bisfluorosulfonylimide (LiFSI), lithium organoborates, or lithium fluoroalkylphosphates and an organic phase such as an alkyl carbonate (e.g. ethylene carbonate (EC), dimethyl carbonate (DEC), propylene carbonate (PC), ethylene methyl carbonate (EMC), fluoroethylene carbonate (FC), vinylene carbonate (VC)), 1,3-propane sulfone, 2-propynyl methanesulfonate, cyclohexylbenzene.

[0053] The separator is a material located between the cathode and anode to keep the two electrodes apart to prevent electrical short circuits while also allowing the transport of ions therethrough. Examples of separator materials include polymers (e.g. polyolefins such as polyethylene, polypropylene and blends thereof). Other materials also present in lithium-ion batteries include the casing and/or auxiliary components, including cathode and anode backing foil/current collectors, including copper and aluminium, along with steel, aluminium and/or plastics which are often used as to house/encase lithium-ion batteries and for other auxiliary functions such as wiring.

[0054] As used herein, the term "electrode material" refers to the combination of cathode and/or anode electrode materials as described above. For example, the electrode material may comprise one or more of lithium metal oxides (cathode material) and graphite (anode material), as referenced above. In some embodiments, the electrode material may comprise a mixed metal material (i.e. a mixed metal oxide material (MMD)).

[0055] The lithium-ion batteries may be end-of-life batteries (e.g. dead/spent or faulty). It will be appreciated that such batteries present little economic value in their current form (e.g. cannot be recharged or sold). In light of the numerous materials making up lithium-ion batteries, there is a need to develop processes to recover a least some of these materials for re-use, recycling and/or commercial sale. The lithium-ion batteries may be intact or may be partially dismantled into one or more smaller components (e.g. casing has been removed). In one embodiment, the lithium-ion batteries have not been subjected to any physical size reduction or dismantling prior introduction to the shredding apparatus described herein. [0056] The present inventors have developed a process in which lithium-ion batteries subjected a shredding step in the presence of an aqueous input stream as described herein can result in the selective separation of values based on the size of particles generated during the shredding step, including recovering finer particles comprising the electrode material separate to coarser larger particulates comprising other values such as copper, aluminium and/or plastic casings and steel. The obtained electrode material is of value and can be commercially sold and/or subjected to further processing to recover one or more metal values such as cobalt and nickel. Additionally, the wet shredding step was found to liberate the electrolyte as part of an aqueous stream which, in some embodiments, could be recycled for use as the aqueous input stream to maintain a more alkaline pH (e.g. less acidic pH) of the wet-environment of the shredding step. By maintaining an alkaline pH during the wet-shredding of the lithium- ion batteries, the generation of one or more halide by-products (e.g. hydrofluoric acid (HF)) can be mitigated and/or neutralised.

[0057] In some embodiments, the process for obtaining an electrode material from lithium-ion batteries, the process comprising the steps of: a) shredding lithium-ion batteries in the presence of a continuous aqueous input stream to obtain a first aqueous slurry stream comprising an aqueous phase, shredded battery particles and an electrolyte, wherein the particles comprise coarser particles of copper, aluminium, plastic and steel and finer particles of the electrode material, and the electrolyte is dissolved or suspended in the aqueous phase of the first aqueous slurry stream; b) separating and obtaining the coarser particles of copper, aluminium, plastic and steel and finer particles of electrode material from the first aqueous slurry stream and producing a first aqueous liquid stream comprising dissolved or suspended electrolyte; and c) recycling at least part of the first aqueous liquid stream comprising dissolved or suspended electrolyte to the shredding at step a) for use in the continuous aqueous input stream.

Wet-shredding [0058] The lithium-ion batteries are subjected to a shredding step in the presence of an aqueous input stream to break up the lithium-ion batteries into shredded battery particles. The shredded battery particles may vary in size. The shredded battery particles may comprise coarser particles and finer particles. This may also be referred to as the “first, primary, or initial shredding step” depending if there are one or more further shredding steps performed in the present process. The shredding of the lithium- ion batteries shears apart the batteries to liberate one or more materials described herein, for example the electrode material and electrolyte. The process comprises introducing a lithium-ion battery feed to a shredder. Referring to Figure 1, a feed of lithium-ion batteries 100 is introduced to the shredding step 104.

[0059] As used herein, the term “shredding” encompasses any suitable physical process designed to break up and dismantle lithium-ion batteries into one or more smaller components. In the context of the present disclosure, shredding also includes crushing and/or milling. Any suitable apparatus capable of shredding the batteries can be used, for example a multi shaft shredder (e.g. a twin/dual shaft shredder or quadruple- shaft shredder), single shaft shredder, granulator, hammer mill, or crusher, which are known to the person skilled in the art. In some embodiments, the shredding step causes a size reduction of the lithium-ion batteries.

[0060] In one embodiment, the shredding step is performed using a multi-shaft shredder, for example a dual/twin shaft shredder. Such shredders comprise a set of blades rotating toward each other to pull material through the centre thereby physically shearing apart the battery into smaller shredded battery particles. The shredded battery particles may comprise a coarser fraction and a finer fraction. For example, the shredded battery particles may comprise a coarser particle fraction comprising copper, aluminium, plastics and steel along with some electrode material also present/trapped within the coarser particle fraction, and a finer particle fraction comprising the electrode material. Aqueous input stream

[0061] The shredding of the lithium-ion batteries is performed in the presence of an aqueous input stream. The aqueous input stream may be a continuous aqueous input stream. It will be appreciated that where the aqueous input stream is under continuous flow, it is introduced into the process with a suitable flow rate sufficient to wet the lithium-ion batteries while they are being shredded.

[0062] It will be appreciated that such “continuous flow” can also include intermittent flow (such as actuated spraying of the aqueous input stream onto the shredding apparatus). The continuous aqueous input stream may also be stopped once the recycling process has completed. In an embodiment, the continuous aqueous input stream is a non-intermittent/non-interrupted flow of the aqueous input stream. In some embodiments, an aqueous input stream will be considered continuous provided that the lithium-ion batteries subjected to the shredding step are sufficiently wetted by the aqueous input stream throughout the duration of the shredding step and/or once one or more values such as the electrode material has been obtained therefrom. The aqueous input stream may be introduced to a housing configured to hold the shredding apparatus and the aqueous input stream as it is introduced (e.g. in flow) to the shredding step. Referring to Figure 1, an aqueous input stream 150 is introduced in flow to the shredding step 104.

[0063] In some embodiments, the aqueous input stream may have a suitable flow rate. In some embodiments, the continuous aqueous input stream may have a flow rate of at least about 0.1, 0.5, 1, 2, 5, 10, 20, 30, 40, 50 or 100 m³/tonne of aqueous input stream per tonne of lithium-ion battery. In some embodiments, the continuous aqueous input stream may have a flow rate of less than about 100, 50, 40, 30, 20, 10, 5, 2, 1, 0.5 or 0.1 m Vtonne of aqueous input stream per tonne of lithium-ion battery. Combinations of these flow rates are also possible, for example, the continuous aqueous input stream may have a flow rate of between about 1 nr'/tonne to about 50 m³/tonne, about 5 rrfVtonne to 40 mVtonne, or about 10 m³/tonne to about 30 rrf'/tonne of aqueous input stream per tonne of lithium-ion battery. [0064] In some embodiments, having a higher flow rate (for example at least about 50 m3/tonne) may provide further advantages such as mitigating fire and fume and dust generation during the shredding process, whilst reducing the overall volume of aqueous liquid required to fully immerse the shredding apparatus under the liquid.

[0065] It will be appreciated that this flow rate only relates to the aqueous input stream and is not intended to limit the flow rates of one or more of the aqueous slurry streams or aqueous liquid streams that are generated by the present process.

[0066] The shredding of lithium-ion batteries liberates the battery electrolyte (e.g. LiPFe), which at temperatures of greater than 70 C, is susceptible to hydrolysis upon exposure to the aqueous input stream or aqueous phase of any resulting slurry stream producing hydrofluoric acid (HF) as shown below:

LiPF₆(aq)+ H₂O(1) = LiF(aq) + 2HF(aq) + POF₃(aq)

[0067] The aqueous input stream may have a suitable pH. In one embodiment, the aqueous input stream has a more alkaline pH (e.g. a less acidic pH), which may provide further advantages such as mitigating any HF which may be generated following exposure of the liberated LiPFe electrolyte with an aqueous solution. In some embodiments, the process further comprises an off-gas treatment step wherein one or more gases (e.g. HF) generated during the shredding at step a) are treated. For example, referring to Figure 1, following the shredding step 104, any residual gases (e.g. HF) that are not mitigated by the input aqueous stream are passed to an off-gas treatment step 600. It will be appreciated that the off-gas treatment step may comprise convention gas cleaning equipment in stages or combination of stages, such as bag filters, wet scrubbers including venturi and packed towers.

[0068] In some embodiments, the aqueous input stream has a pH of at least 6, 7, 8, 9, 10, 11 or 12. In some embodiments, the aqueous input stream has a pH of less than about 12, 11, 10, 9, 8, 7 or 6. Combinations of these pH values are also possible, for example, the aqueous input stream may have a pH of between about pH 6 to about pH 12, pH 7 to about 11 or about pH 8 to about pH 10. In some embodiments, the pH of the aqueous input stream may also be maintained/controlled by the electrolyte which is liberated from the lithium-ion battery during the shredding process and recycled to the shredding at step a) for use in the continuous aqueous input stream (discussed below).

[0069] In some embodiments, the aqueous input stream comprises water. In some embodiments, the aqueous input stream does not comprise lime (e.g. does not comprise CaO or Ca(OH)2 (i.e. hydrated lime)). In some embodiments the aqueous input stream does not comprise a solvent, for example does not comprise one or more of n-methyl-2- pyrrolidone (NMP), dimethylformamide (DMF), ethyl acetate (EtOAc), isopropanol (IP A), acetone, dimethyl sulfoxide (DMSO), or diethylformamide (DEF).

[0070] The aqueous input stream may also have a suitable temperature. In some embodiments, the temperature of the aqueous input stream is less 70, 60, 50, 40, 30, 20, 10 or 5 °C. Combinations of these temperature ranges are also possible, for example, the temperature of the aqueous input stream may be between about 10°C to about 70°C. In some embodiments, the temperature of the aqueous input stream may also be maintained/controlled by removing heat which is liberated from the lithium-ion battery during the shredding process and recycled to the shredding at step a). Any suitable apparatus capable of removing heat can be used, for example heat exchangers or forced evaporation devices, which are known to the person skilled in the art.

[0071] In some embodiments, the process comprises the recycling of one or more aqueous liquid streams (e.g. at least part of the first aqueous liquid stream) back in to the wet-shredding step for use in the aqueous input stream. Depending on the volume of liquid being recycled a closed-loop continuous flow of the input stream may be generated. In this embodiment, it will be appreciated that an external supply of the aqueous make-up stream is not always required to maintain a continuous flow owing to the recycling of one or more aqueous liquid streams generated downstream (e.g. at least part of the first aqueous liquid stream 120 and optionally part of the second aqueous liquid stream 240). In other embodiments, an external aqueous make-up stream may be added to the recycled aqueous liquid stream. For example, referring to Figure 1, an aqueous make-up stream 145 may be introduced into the aqueous input stream. It will be appreciated that the external aqueous make-up stream could alternately be added directly to the shredding process 104 as a separated stream (not shown) or directly to the dewatering and classification 115 (not shown) or any combination of these locations.

[0072] In some embodiments, the aqueous make-up stream comprises water or another suitable aqueous solution.

First aqueous slurry stream

[0073] Owing to the presence of the aqueous input stream, the shredding of the lithium-ion batteries produces a first aqueous slurry stream comprising an aqueous phase and shredded battery particles. The shredded battery particles may vary in size (for example range from finer smaller particles of electrode material up to coarser larger particles of copper, aluminium, plastic and steel). The aqueous phase of the first aqueous slurry stream is generated from the aqueous input stream used during the shredding at step a). Along with comprising the shredded battery particles, the first aqueous slurry stream comprises an electrolyte, wherein the electrolyte is dissolved or suspended in the aqueous phase of the first aqueous slurry stream.

[0074] The first aqueous slurry stream comprises shredded battery particles. The term “particle” (also referred to as “particulate”) refers to the form of discrete solid units. The units may take the form of flakes, fibres, agglomerates, granules, powders, spheres, pulverized materials or the like, as well as combinations thereof. The particles may have any desired shape including, but not limited to, cubic, rod like, polyhedral, spherical or semi-spherical, rounded or semi-rounded, angular, irregular, and so forth.

[0075] The first aqueous slurry stream has a solids concentration. In some embodiments, the first aqueous slurry stream has a solids concentration of at least about 0.5, 1, 1.5, 2, 2.5, 3, 4, 5, 10, 15, 20, 25 30, 40, 50, 60, 70, 80, 90 or 95% w/w based on the total weight of the slurry stream. In some embodiments, the first aqueous slurry stream has a solids concentration of less than about 95, 90, 80, 70, 60, 50, 40 or 30, 25, 20, 15, 10, 5, 4, 3, 2.5, 2, 1.5, 1 or 0.5% w/w based on the total weight of the slurry stream. Combinations of these % w/w values are also possible, for example between about 1% w/w to about 95% w/w, about 2% w/w to about 80% w/w, about 3% w/w to about 70% w/w, e.g. 5% w/w to about 50% w/w. It will be appreciated that the solids concentration will vary depending on the flow rate of the aqueous input stream, where a higher flow rate (e.g. 50 m³/tonne) can result in a lower solids concentration and a lower flow rate (e.g. 0.1 nr'/tonne) can result in a higher solids concentration.

[0076] The shredded battery particles may have an average particle size. The average particle size is taken to be the cross-sectional diameter across a particle. For non- spherical particles, the particle size is taken to be the distance corresponding to the longest cross-section dimension across the particle. In some embodiments, first aqueous slurry stream comprises shredded battery particles that vary in average size.

[0077] In some embodiments, the shredded battery particles have an average particle size of between about 1 pm to about 50,000 pm, for example at least about 1, 10, 50, 100, 150, 200, 250, 500, 1,000, 2,000, 5,000, 10,000, 15,000, 20,000, 25,000 or 50,000 pm. In some embodiments, the shredded battery particles have an average particle size of less than about 50,000, 25,000, 20,000, 15,000, 10,000, 5,000, 2,000, 1,000, 500, 250, 200, 150, 100, 50, 10 or 1 pm. Combinations of these sizes are also possible, for example between about 5 pm to about 10,000 pm. In some embodiments, the shredded battery particles have a polydisperse size distribution (e.g. a size distribution that varies greater than 5%). In some embodiments, the shredded battery particles have a particle size distribution (PSD), wherein 90% of the particles (P90) have a particle size of less than about 25,000, 20,000, 15,000 or 10,000 pm or wherein 80% of the particles (Pso) have a particle size of less than about 20,000, 15,000, 10,000 or 5,000 pm, or wherein 50% of the particles (P50) have a particle size of less than about 15,000, 10,000, 5,000 or 2,000 pm. In one embodiment, the further shredding of the second aqueous slurry stream may result in a size-reduced slurry stream having a particle size distribution (PSD), wherein 90% of the particles (P90) have a particle size of less than about 10,000 pm. [0078] In some embodiments, the shredded battery particles comprises coarser particles and finer particles. In some embodiments, the finer particles have an average particle size of less than about 500, 450, 400, 350, 300, 200, 150, 100, 70, 50, 20 or 10 pm. In some embodiments, the finer particles have an average particle size of at least about 10, 20, 50, 70, 100, 150, 200, 300, 350, 400, 450 or 500 pm. Combinations of these sizes are also possible, for example between about 10 pm to about 500 pm, or about 100 pm to about 400 pm.

[0079] In some embodiments, the average particle size of the coarser particles is at least about 500, 1,000, 2,000, 5,000, 10,000, 15,000, 20,000, 25,000 or 50,000 pm. In some embodiments, the average particle size of the coarser particles is less than about 50,000, 25,000, 15,000, 10,000, 5,000, 2,000 or 1,000 pm. Combinations of these sizes are also possible, for example between about 1,000 pm to about 20,000 pm, e.g. about 10,000 pm.

[0080] The average particles size and/or PSD can be measured by any conventional method, including laser diffraction, electron microscopy, dynamic light scattering, optical microscopy or size exclusion methods (such as wet or dry graduated mesh screens or filters).

[0081] At least some of the shredded particles comprise the electrode material. For example, the finer particles may comprise electrode material. In some embodiments, at least one electrode material is selected from a cathode material and an anode material. The electrode material, cathode material and anode material are described herein. Other materials may also be present in one or more of the shredded battery particles. For example, coarser particles may comprise one or more of copper, aluminium, plastic and steel materials.

[0082] In some embodiments, the first aqueous slurry stream is subjected to further shredding to reduce the average particle size of the shredded battery particles prior to separating the particles at step b). For example, the first aqueous slurry stream may be returned or partially returned to the shredding step a) for further shredding, or alternatively may be introduced to a separate shredding apparatus described herein.

[0083] Referring to Figure 1, following the shredding step 105, a first aqueous slurry stream is produced 139 comprising shredded battery particles.

First and second aqueous liquid streams

[0084] Separating the shredded battery particles from the first aqueous slurry stream produces a first aqueous liquid stream and, in some embodiments, also produces a second aqueous liquid stream. The first and second aqueous liquid streams each comprise dissolved or suspended electrolyte as it is liberated from the lithium-ion batteries during wet-shredding.

[0085] The electrolyte may comprise one or more of hexafluorophosphate (LiPFe), lithium tetrafluoroborate (LiBF4), lithium perchlorate (LiClOi), lithium hexafluoroarsenate monohydrate (LiAsFe), lithium trifluoromethanesulfonate (LiCFsSCh), lithium bis(bistrifluoromethanesulfonyl)imide (LiTFSI), lithium bisfluorosulfonylimide (LiFSI), lithium organoborates, or lithium fluoroalkylphosphates and an organic compound such as an alkyl carbonate (e.g. ethylene carbonate (EC), dimethyl carbonate (DEC), propylene carbonate (PC), ethylene methyl carbonate (EMC), fluoroethylene carbonate (FC), vinylene carbonate (VC)), ethylene glycol, 1,3-propane sulfone, 2-propynyl methanesulfonate, cyclohexylbenzene.

[0086] In some embodiments, the first and/or second aqueous liquid streams do not comprise a solvent for example does not comprise one or more of n-methyl-2- pyrrolidone (NMP), dimethylformamide (DMF), ethyl acetate (EtOAc), isopropanol (IP A), acetone, dimethyl sulfoxide (DMSO), or diethylformamide (DEF).

[0087] In some embodiments, at least part of the first aqueous liquid stream comprising dissolved or suspended electrolyte is recycled to the wet-shredding step for use in the continuous aqueous input stream. By recycling at least part of the first aqueous liquid stream into the aqueous input stream, a more alkaline pH (e.g. less acidic pH) of the wet-environment of the shredding step was maintained. By maintaining an alkaline pH during the wet-shredding of the lithium-ion batteries, the generation of one or more halide by-products (e.g. hydrofluoric acid (HF)) can be mitigated. For example, referring to Figure 1, part of the first liquid stream 120 can be recycled back for use in the continuous aqueous input stream 150.

[0088] Referring to Figure 1, by way of example, separating the shredded battery particles from the first aqueous slurry stream 139 produces a first aqueous liquid stream 120 and part of the first aqueous liquid stream 120 is recycled back for use in the continuous input stream. Additionally, in this example, part of the first aqueous liquid stream 120 is also treated to recover one or more electrolyte compounds 500. It will be appreciated that in this example, the recycled and treated aqueous liquid streams are both part of the first aqueous liquid stream.

[0089] In some embodiments, the separating and obtaining the shredded battery particles from the first aqueous slurry stream produces a first and second aqueous liquid stream. It will be understood that these streams are produced as separate streams and the second aqueous liquid stream is not a “run-off’ stream from the first aqueous liquid stream. For example, referring to Figure 2, the separating and obtaining the coarser and finer particles at step b) may comprise dewatering and classifying 115 the first aqueous slurry stream to produce the first aqueous liquid stream 120. A second aqueous liquid stream 240 may then be produced following the separating of the particles from the aqueous slurry stream 225 generated downstream following the dewatering and classifying step. It will be appreciated that in this example, the first and second aqueous liquid streams may each comprise different amounts of dissolved or suspended electrolyte (e.g. comprise different concentrations of lithium, phosphate and fluorine etc.)

[0090] In some embodiments, it will be appreciated that at the beginning of the process, until such recycling step has occurred, the aqueous input stream does not comprise any dissolved or suspended electrolyte. Once part of the first aqueous liquid stream is generated and recycled back to the wet-shredding step (e.g. initial shredding step) for use in the aqueous input stream, any generation of halide by-products (e.g. HF) during the continued shredding of the lithium-ion battery feed can be mitigated. While the aqueous input stream can mitigate the generation of HF, the process may further comprise an off-gas treatment step described above to treat one or more gases generated during the shredding of the lithium-ion batteries.

[0091] In some embodiments, the first and/or second aqueous liquid stream comprising dissolved or suspended electrolyte has a pH of at least 6, 7, 8, 9, 10, 11 or 12. In some embodiments, the first aqueous stream has a pH of less than about 12, 11, 10, 9, 8, 7 or 6. Combinations of these pH values are also possible, for example, the first aqueous and/or second aqueous liquid streams may have a pH of between about pH 6 to about pH 12, about pH 7 to about pH 11 or about pH 8 to about pH 10.

[0092] In some embodiments, the recycling of part of the first aqueous liquid stream comprising dissolved or suspended electrolyte is provided to maintain the pH of the continuous aqueous input stream of at least 6, 7, 8, 9, 10, 11 or 12. In some embodiments, the recycling of part of the first aqueous liquid stream comprising dissolved or suspended electrolyte is provided to maintain the pH of the continuous aqueous input stream of less than about 12, 11, 10, 9, 8, 7 or 6. Combinations of these pH values are also possible, for example, of between about pH 6 to about pH 12, about pH 7 to about pH 11 or about pH 8 to about pH 10.

[0093] In some embodiments, the concentration of lithium in the first and/or second aqueous liquid stream comprising dissolved or suspended electrolyte is at least about 100, 200, 300, 500, 1,000, 1,500, 2,000, 3,000, 4,000 or 5,000 mg/L based on the volume of the aqueous liquid stream. In some embodiments, the concentration of lithium in the first and/or second aqueous liquid stream comprising dissolved or suspended electrolyte is less than about 5,000, 4,000, 3,000, 2,000, 1,500, 1,000, 500, 300, 200 or 100 mg/L based on the volume of the aqueous liquid stream. Combinations of these concentration values are also possible, for example between about 200 mg/L to about 10,000 mg/L, about 200 mg/L to about 5,000 mg/L, about 700 mg/L to about 6,000 mg/L, about 700 mg/L to about 4,000 mg/L or about 1,500 mg/L to about 5,000 mg/L, about 1,500 mg/L to about 3,000 mg/L based on the volume of the aqueous liquid stream.

[0094] In some embodiments, the concentration of fluoride in the first and/or second aqueous liquid stream comprising dissolved or suspended electrolyte is at least about 100, 200, 300, 500, 1,000, 1,500, 2,000, 3,000, 4,000 or 5,000 mg/L based on the volume of the aqueous liquid stream. In some embodiments, the concentration of fluoride in the first and/or second aqueous liquid stream comprising dissolved or suspended electrolyte is less than about 5,000, 4,000, 3,000, 2,000, 1,500, 1,000, 500, 300, 200 or 100 mg/L based on the volume of the aqueous liquid stream. Combinations of these concentration values are also possible, for example between about 100 mg/L to about 1,000 mg/L, about 700 mg/L to about 4,000 mg/L or about 1,500 mg/L to about 3,000 mg/L based on the volume of the aqueous liquid stream.

[0095] In some embodiments, the concentration of phosphorous in the first and/or second aqueous liquid stream comprising dissolved or suspended electrolyte is at least about 100, 200, 300, 500, 1,000, 1,500, 2,000, 3,000, 4,000 or 5,000 mg/L based on the volume of the aqueous liquid stream. In some embodiments, the concentration of phosphorous in the first and/or second aqueous liquid stream comprising dissolved or suspended electrolyte is less than about 5,000, 4,000, 3,000, 2,000, 1,500, 1,000, 500, 300, 200 or 100 mg/L based on the volume of the aqueous liquid stream. Combinations of these concentration values are also possible, for example between about 100 mg/L to about 1,000 mg/L, about 700 mg/L to about 4,000 mg/L or about 1,500 mg/L to about 3,000 mg/L based on the volume of the aqueous liquid stream.

[0096] It will be appreciated that while the majority of the solids content (e.g. particles) has been separated from the first and/or second aqueous liquid stream, the first and/or second aqueous liquid stream may have a solids concentration owing to the presence of one or more particles/material that were not separated therefrom. In some embodiments, the first and/or second aqueous liquid stream has a solids concentration of less than about 5%, 4%, 3%, 2%, 1%, 0.5%, 0.1%, 0.01% or 0.001% w/w based on the total weight of the aqueous liquid stream.

[0097] In some embodiments, at least part of the first and/or second aqueous liquid stream comprising dissolved or suspended electrolyte is further treated to remove (i.e. recover) one or more inorganic and organic species present in the first aqueous liquid stream (described below). Referring to Figure 1, part of the first aqueous liquid stream 120 can be further treated 500 to remove one or more inorganic and organic species present in the aqueous stream, such as fluoride, phosphate, and lithium 554 producing a treated aqueous stream 570 which can be recycled as an input back into the process. Referring to Figure 2, the second aqueous liquid stream 240 can be further treated ( e.g. 504, 530, 565) to remove one or more inorganic and organic species present in the aqueous stream.

[0098] In some embodiments, at least part of the second aqueous liquid stream comprising dissolved or suspended electrolyte may optionally be recycled to the wetshredding step for use in the continuous aqueous input stream. For example, referring to Figure 2, part of the second aqueous liquid stream is recycled to the initial shredding step (see optional dashed line 240).

Dewatering and classifying the first aqueous slurry stream

[0099] In some embodiments, the first aqueous slurry stream may be further processed to liberate any electrode material that may be trapped within larger coarser shredded battery particles, liberate any electrolyte that may be trapped within the particles, and/or separate out larger material components such as copper, aluminium, plastic and steel.

[0100] In some embodiments, the separating and obtaining the particles at step b) comprises: bl) dewatering and classifying the first aqueous slurry stream comprising the shredded battery particles based on particle size to produce a second aqueous slurry stream comprising coarser particles, a third aqueous slurry stream comprising finer particles, and the first aqueous liquid stream.

[0101] As used herein, the term “dewatering” essentially refers to the removal of water or aqueous solution from a slurry. Various dewatering methods can be utilised, including wet-classification, filtration or solid liquid separation process such as wetscreening.

[0102] As used herein, the term “classifying” or “classification” refers to the process of separating a slurry comprising a mixture of particles into two product streams (e.g. slurry streams) based on particle size. Classifying involves separating finer particles from coarser particles and lighter particles from heavier particles. The two product streams obtained from classification usually comprise i) a dewatered aqueous slurry stream comprising coarser particles, and ii) an aqueous slurry stream comprising finer particles.

[0103] As will be understood by the person skilled in the art, classification is usually performed on the basis of particle size, shape or density. In particular, classification makes use of the different rate of movement that particles of different sizes and densities suspended in the slurry have, and how they are differentially affected by imposed forces such as gravity thereby collecting the different streams comprising coarse or fine particles as they move to different regions.

[0104] In some embodiments, the dewatering and classification of the first aqueous slurry stream is performed using a screw classifier (also referred to as a spiral classifier). Other suitable devices used to dewater and classify the first aqueous slurry stream include up current classifier, reflux classifier, cone classifiers, double cone classifiers, gravity settling tanks, rake classifiers, hydrocyclone classifiers and dense media separation. Alternatively, the dewatering and classifying may be performed using a suitable screen and thickener (e.g. wet-screening at about 500 pm). [0105] In one embodiment, the dewatering and classifying of the first aqueous slurry stream is performed using a screw classifier. Screw classifiers comprise a semi cylindrical trough (a trough which is semi-circular in cross-section) inclined to the horizontal. In some embodiments, slurry is fed continuously near the middle of the trough. The screw classifier moves the coarser heavier solids which settle to the bottom upward along the floor of the trough towards the top of the trough and out an opening in the form of a dewatered aqueous slurry stream comprising the coarser particles. In contrast, the finer particles do not have time to settle and are carried out with the overflow liquid as part of an aqueous slurry stream comprising the finer particles.

[0106] In some embodiments, one or more gases (e.g. HF) generated during the classification and dewatering step are treated. For example, referring to Figure 2, during the classification and dewatering step 115, any residual gases (e.g. HF) that are not mitigated by the input aqueous liquid stream are passed to an off-gas treatment step 600. It will be appreciated that the off-gas treatment step may comprise gas cleaning equipment in stages or combination of stages, such as bag filters, wet scrubbers including venturi and packed towers.

[0107] In some embodiments, the first aqueous liquid stream is produced from the dewatering and classifying of the first aqueous slurry stream. Referring to Figure 2, following the dewatering and classification 115, the first aqueous liquid stream is produced 120 along with the second aqueous slurry stream 130 and third aqueous slurry stream 125. The first aqueous liquid stream comprises dissolved or suspended electrolyte as described herein. In some embodiments, at least part of the first aqueous liquid stream comprising dissolved or suspended electrolyte may be recycled to the shredding at step a) for use in the continuous aqueous input stream.

[0108] The pH, electrolyte, electrolyte concentration (e.g. lithium, phosphorous, fluorine concentration), pH maintenance of the input stream, and solids concentration described above in relation the first and/or second aqueous liquid streams are also applicable to the second aqueous liquid stream described here in relation to the classifying and dewatering step. Second aqueous slurry stream and further shredding

[0109] The dewatering and classifying of the first aqueous slurry stream comprising the shredded battery particles produces a second aqueous slurry stream comprising coarser particles. The coarser particles have a larger average particle size compared to the finer particles in the third aqueous slurry stream. The second aqueous slurry stream comprising finer particles may also be referred to as a coarser particle stream.

[0110] In some embodiments, the average particle size of the coarser particles in the second aqueous slurry stream is at least about 200, 500, 1,000, 2,000, 5,000, 10,000, 15,000, 20,000, 25,000 or 50,000 pm. In some embodiments, the average particle size of the coarser particles in the second aqueous slurry stream is less than about 50,000, 25,000, 15,000, 10,000, 5,000, 2,000, 1,000, 500 or 200 pm. Combinations of these sizes are also possible, for example between about 500 pm to about 20,000 pm, e.g. about 10,000 pm.

[0111] Owing to the dewatering and classification step, the second aqueous slurry stream has a higher solids concentration compared to the solids concentration of the first aqueous slurry stream. In some embodiments, the second aqueous slurry stream has a solids concentration at least about 50, 60, 70, 80, 85, 90 or 99% w/w based on the total weight of the slurry stream. In some embodiments, the second aqueous slurry stream has a solids concentration of less than about 99, 90, 85, 80, 70, 60 or 50% w/w based on the total weight of the slurry stream. Combinations of these % w/w values are also possible, for example between about 60% w/w to 99% w/w, about 70% w/w to about 95% w/w, e.g. 80% w/w to about 95% w/w.

[0112] At least some of the coarser particles comprise electrode material. In some embodiments, at least one electrode material is selected from a cathode material and an anode material. The electrode material, cathode material and anode material are described herein. Along with comprising electrode material, the coarser particles may also comprise one or more additional materials including copper, aluminium, plastic and steel. Coarser particles comprising steel may also be referred to as magnetic particles or a magnetic susceptible fraction.

[0113] The second aqueous slurry stream may be subjected to further shredding steps to reduce the average particle size of the coarser particles therein. In some embodiments, the process further comprises step b2) subjecting the second aqueous slurry stream comprising the coarser particles to further shredding to reduce the average particle size of the coarser particles. By further shredding the coarser particles, electrode material trapped within the particles can be liberated and separated from other materials such as copper, aluminium, plastic and steel resulting in a higher purity end product, for example cathode and anode material with minimal contamination. This may also be referred to as the “second, further, or secondary shredding step”. Referring to Figure 2, the second aqueous slurry stream 130 is subjected to a further shredding step 135.

[0114] The further shredding of the second aqueous slurry stream results in a size- reduced second aqueous slurry stream. The size-reduced second aqueous slurry stream comprises reduced sized coarser particles. In some embodiments, the further shredding of the second aqueous slurry stream may result in a size-reduced aqueous slurry stream having a particle size distribution (PSD), wherein 90% of the particles (P90) have a particle size of less than about 10,000, 8,000, 7,000, 6,000 or 5,000 pm, or wherein 80% of the particles (Pso) have a particle size of less than about 8,000, 7,000, 6,000, 5,000 or 4,000 pm, or wherein 50% of the particles (P50) have a particle size of less than about 5,000, 4,000, 3,000, 2,000, 1,000 or 500 pm. In one embodiment, the further shredding of the second aqueous slurry stream may result in a size-reduced aqueous slurry stream having a particle size distribution (PSD), wherein 90% of the particles (P90) have a particle size of less than about 10,000 pm.

[0115] In some embodiments, the further shredding reduces the average particle size of the coarser particles to less than about 5,000, 4,000, 3,000, 2,000, 1,000, 750, 500, 450, 400, 350, 300, 200, 150, 100, 70, 50, 20 or 10 pm. In some embodiments, the finer particles have an average particle size of at least about 10, 20, 50, 70, 100, 150, 200, 300, 350, 400, 450, 500, 750, 1,000, 2,000, 3,000, 4,000 or 5,000 pm. Combinations of these sizes are also possible, for example between about 100 pm to about 2,000 pm, or about 500 pm to about 1,000 pm.

[0116] In some embodiments, the shredding apparatus used in this further shredding step may be the same or different shredding apparatus to that used in the initial or first shredding step of the lithium-ion batteries. In one embodiment, the shredding apparatus used in the further shredding step may be different to the shredding apparatus used in the shredding at step a). For example, the further shredding may be conducted using a single shaft shredder with a grate discharge or dual/twin shaft or multiple single shaft shredder as described herein in the absence or presence of an continuous flow aqueous input stream.

[0117] In some embodiments, the further shredding step is performed in the absence of a continuous aqueous input stream. For example, the further shredding step is substantially “dry” when compared to the initial shredding step which is performed in the presence of an aqueous input stream. The term “dry” is used to refer to the absence of an continuous flow aqueous input stream as opposed to describing the moisture content of the second aqueous slurry stream.

[0118] In some embodiments, the further shredding step is performed in the presence of a second continuous aqueous input stream. Referring to Figure 2, a second aqueous input stream 151 can be introduced in-flow to the further shredding step 135. For example the second continuous aqueous input stream may have a flow rate of at least about 0.1, 0.5, 1, 2, 5, 10, 15, 20, 30, 40, 50 or 100 m³/tonne of second aqueous input stream per tonne of solids in the second aqueous slurry stream (130). In some embodiments, the continuous aqueous input stream may have a flow rate of less than about 100, 50, 40, 30, 20, 15, 10, 5, 2, 1, 0.5 or 0.1 m³/tonne of second aqueous input stream per tonne of solids in the second aqueous slurry stream. Combinations of these flow rates are also possible, for example, the second continuous aqueous input stream may have a flow rate of between about 0.1 m³/tonne to about 50 m³/tonne, about 5 nr'/tonne to 40 m tonne, or about 10 m³/tonne to about 30 m tonne of second aqueous input stream per tonne of solids in the second aqueous slurry stream.

[0119] In some embodiments, the further shredding step includes multiple shredding apparatus in series. For example, using the single or multiple of same or different apparatus to that used in the initial or first shredding step of the lithium-ion batteries followed by milling or impact crushing apparatus. In one embodiment, the multiple types of shredding apparatus can be separated by dewatering and classification stages.

[0120] In some embodiments the further shredding step includes classification and dewatering stage to recover fine material. Referring to Figure 2 recovered fine material (141) is combined with the third aqueous slurry stream (125).

[0121] In some embodiments, one or more gases (e.g. HF) generated during further shredding step are treated. For example, referring to Figure 2, any residual gases (e.g. HF) generated during the further shredding step 135 are passed to an off-gas treatment step 600. It will be appreciated that the off-gas treatment step may comprise gas cleaning equipment in stages or combination of stages, such as bag filters, wet scrubbers including venturi and packed towers.

[0122] In some embodiments, the particles may be separated and obtained from the size-reduced second aqueous slurry stream.

Third aqueous slurry stream

[0123] The dewatering and classifying of the first aqueous slurry stream comprising the shredded battery particles produces a third aqueous slurry stream comprising finer particles. The finer particles have a smaller average particle size compared to the coarser particles in the second aqueous slurry stream. The third aqueous slurry stream comprising finer particles may also be referred to as a finer particle stream. [0124] The finer particles comprise electrode material. In some embodiments, at least one electrode material is selected from a cathode material and an anode material. The electrode material, cathode material and anode material are described herein.

[0125] In some embodiments, the finer particles have an average particle size of less than about 1,000, 750, 500, 450, 400, 350, 300, 200, 150, 100, 70, 50, 20, 10, 5 or 1 pm. In some embodiments, the finer particles have an average particle size of at least about 1, 5, 10, 20, 50, 70, 100, 150, 200, 300, 350, 400, 450, 500, 750 or 1,000 pm. Combinations of these sizes are also possible, for example between about 1 pm to about 1,000 pm, or about 5 pm to about 750 pm.

[0126] In some embodiments, the third aqueous slurry stream has a particle size distribution (PSD), wherein 90% of the particles (P90) have a particle size of less than about 500, 450, 400, 350, 300 or 200 pm, or wherein 80% of the particles (Pso) have a particle size of less than about 400, 350, 300, 200, 150 or 100 pm, or wherein 50% of the particles (P50) have a particle size of less than about 300, 200, 150, 100, 70 or 50 pm. In one embodiment, the third aqueous slurry stream has a particle size distribution (PSD), wherein 90% of the particles (P90) have a particle size of less than 300 pm.

[0127] In some embodiments, the third aqueous slurry stream comprises at least about 1, 2, 3, 4, 5, 6, 8, 10, 12, 15, 20 or 30% of the total electrode material present in the first aqueous slurry stream. In some embodiments, the third aqueous slurry stream comprises less than about 30, 20, 15, 12, 10, 8, 6, 5, 4, 3, 2 or 1% of the total electrode material present in the first aqueous slurry stream. Combination of these values are also possible, for example between about 1% to about 30%, e.g. about 1% to about 20% of the total electrode material present in the first aqueous slurry stream.

[0128] Owing to the dewatering and classification step, the third aqueous slurry stream has a lower solids concentration compared to the solids concentration of the first aqueous slurry stream. In some embodiments, the third aqueous slurry stream has a solids concentration at least about 1, 2, 3, 4, 5, 8, 10, 15, 20, 25, 30, 40 or 50% w/w based on the total weight of the slurry stream. In some embodiments, the third aqueous slurry stream has a solids concentration of less than about 50, 40, 30, 25, 20, 15, 10, 8, 5, 4, 3, 2 or 1% w/w based on the total weight of the slurry stream. Combinations of these % w/w values are also possible, for example between about 1% w/w to about 30% w/w, e.g. 5% w/w to about 50% w/w, or about 5% to about 20% w/w.

[0129] In some embodiments, the particles may be separated and obtained from the third aqueous slurry stream.

[0130] In some embodiments, the process comprises the step b3) combining the size- reduced second aqueous slurry stream with the third aqueous slurry stream to obtain the first aqueous slurry stream and separating the particles therefrom. For example, referring to Figure 2, the third aqueous slurry stream 125 is combined with the size- reduced second aqueous slurry stream 140 to form first aqueous slurry stream and then separating the particles 210 and 225 therefrom and producing to produce a second aqueous liquid stream 240. At least part of the second aqueous liquid stream 240 may be treated to recover one or more electrolyte compounds (e.g. 504, 530, 565) and optionally at least part of the second aqueous liquid stream 240 may be recycled as part of the input stream 150 to the initial wet-shredding step 105. Optionally the third aqueous slurry stream can be combined with the undersized second aqueous slurry stream 220 (not shown) where coarser particles comprising copper, aluminium, plastic and steel have already been removed prior to solid liquid separation 225 (not shown).

Washing and attritioning the shredded particles

[0131] In some embodiments, the shredded particles in the first aqueous slurry stream are subjected to a washing and/or attritioning step prior to separating the particles therefrom at step b). Such a washing and/or attritioning step may liberate electrolyte and/or electrode material trapped within the shredded battery particles. During the washing and/or attritioning step, the shredded battery particles impact one another which “cleans” the particles and liberated electrode material. The washing step may comprise adding a suitable aqueous wash solution to the first aqueous slurry stream. The aqueous wash solution may be water. Referring to Figure 2, the shredded particles are subjected to a washing and attritioning step 200. An aqueous wash solution 275 may comprise part of the first aqueous liquid stream 235 and/or may be a make-up wash stream 270. In some embodiments, the aqueous wash solution does not comprise a solvent, for example does not comprise a stripping solvent, e.g. does not comprise one or more of n-methyl-2-pyrrolidone (NMP), dimethylformamide (DMF), ethyl acetate (EtOAc), isopropanol (IP A), acetone, dimethyl sulfoxide (DMSO), or diethylformamide (DEF).

[0132] According to at least some embodiments or examples described herein, by washing and attritioning the shredded battery particles in the presence of the coarser particles (such as the magnetic steel particles), further advantages can be provided, including improved liberation and recovery of electrode materials without the use of toxic stripping solvents. In one embodiment, the shredded particles in the first aqueous slurry stream are subjected to a washing and/or attritioning step in the presence of steel particles (e.g. the magnetic fraction). By washing and/or attritioning the shredded particles in the presence of the larger steel fraction, further advantages can be provided according to at least some embodiments or examples described herein, such as the shredded particles can collide with the steel particles during washing and/or attritioning which can assist in additional electrode material being liberated. By not removing the steel particles from the first aqueous slurry stream prior to the washing and/or attritioning step, liberation of electrode material from the shredded particles can be achieved without the need for toxic stripping solvents, according to some embodiments or examples described herein.

[0133] Following any washing step, the washate may be recycled back for use as part of the aqueous input stream or the aqueous wash solution. Any suitable device may be used to wash/attrition the shredded battery particles, for example a washing drum, trommel and/or an agitated attritioning cell.

[0134] In some embodiments, the amount of aqueous wash solution added during the washing and/or attritioning step provides the first aqueous slurry stream with a solids concentration of at least about 5, 10, 15, 20, 25, 30, 35, 40, 45, 50 or 60% w/w based on the total weight of the first aqueous slurry stream. In some embodiments, the amount of aqueous wash solution added during the washing and/or attritioning step provides the first aqueous slurry stream with a solids concentration of less than about 60, 50, 45, 40, 35, 30, 25, 20, 15, 10 or 5% w/w based on the total weight of the first aqueous slurry stream. Combinations of these values are also possible, for example between about 5% w/w to about 70% w/w, about 5% w/w to about 50% w/w, or about 10% w/w to about 50% w/w.

Separating and obtaining particles comprising electrode material

[0135] The shredded battery particles are separated (e.g. classification) from the first aqueous slurry stream. In some embodiments, the process comprises separating and obtaining the coarser particles of copper, aluminium, plastic and steel and finer particles of the electrode material from the first aqueous slurry stream.

[0136] The separated particles may be obtained as single particle stream comprising the particles. Alternatively, the separated particles may be obtained as independent streams of separated particles (e.g. a coarser particle stream and a finer particle stream), which will be appreciated is different from the first aqueous slurry stream and the first and/or second aqueous liquid streams described herein. For example, the coarser particles may be separated as a second aqueous slurry stream described herein, and the finer particles may be separated as a third aqueous slurry stream described herein. One or more aqueous liquid streams (e.g. a first aqueous liquid stream comprising dissolved or suspended electrolyte) may also be produced as a separate stream(s) as result of and in addition to the separating of the coarser and finer particles from the first aqueous slurry stream.

[0137] In some embodiments, the separating and obtaining of the coarser and finer particles at step b) comprises separating and obtaining the coarser particles of copper, aluminium, plastic and steel from the first aqueous slurry stream to obtain a separated first aqueous slurry stream comprising the finer particles of electrode material, and subsequently separating and obtaining the finer particles of electrode material from the separated first aqueous slurry stream and producing the first aqueous liquid stream. In some embodiments, the separating and obtaining of the coarser and finer particles at step b) also produces a second aqueous liquid stream.

[0138] It will be understood that in this embodiment the second aqueous liquid stream is not a “run-off’ stream of the first aqueous liquid stream described herein, but rather represents a separate aqueous liquid stream.

[0139] The particles may be separated by any conventional separation or classification technique, including wet screening or wet-size separation, solid liquid separation, gravity separation, screw classifying, hydrocylcones and other suitable physical separation techniques/devices. For example, wet-screening involves the physical sizing using openings through which particles will either pass through or not. Examples of suitable screens include vibrating screens, multideck screens, sieve bends, static screens, grizzly screens and trommel screens.

[0140] In some embodiments, the separating and obtaining the coarser and finer particles at step b) comprises a wet-size separation step to remove coarser particles comprising copper, aluminium, plastic and steel from the first aqueous slurry stream and produces a separated first aqueous slurry stream comprising finer particles wherein the finer particles comprise the electrode material.

[0141] In some embodiments, the shredded battery particles can be separated from the first aqueous slurry stream via wet-size separation below about 1,000, 800, 600, 500, 400, 300, 250, 200, 150 or 100 pm, including combinations thereof, for example between about 500 pm to about 150 pm, or about 300 pm to about 150 pm to obtain particles comprising the electrode material (e.g. screened undersize particles). The particles comprising the electrode material may undergo a solid liquid separation step to obtain the electrode material.

[0142] In some embodiments, following the separating of the particles comprising the electrode material at step b) and prior to any solid liquid separation step, the separated particles comprising the electrode material undergo gravity separation to separate the cathode material from the anode material (see for example Figure 5, 245), for example using a gravity separation device, such as spiral, jig, up current classifier, reflux classifier, and dense media separation or high-g separator such as a Knelson concentrator, centrifuge or multi gravity separator. In this embodiment, particles comprising the cathode material report to the heavy gravity product, which may be separated and dewatered to recover the cathode material as filter cake for a sale as a product. The particles comprising the anode material report to the light gravity product, may subsequently undergo a solid liquid separation as described herein to recover the anode material as a filter cake for sale as a product. Any recovered aqueous liquid stream is optionally recycled for use upstream in one or more shredding, washing, separation and attritioning steps as described herein, or further treated to remove any captured electrolyte.

[0143] If present, any larger fraction (e.g. screened oversize coarser particles) obtained during the size separation step may be further processed to recover one or more additional materials, such as copper, aluminium, plastic and steel. In some embodiments, larger coarser particles comprising copper, aluminium, plastic and steel are subjected to a magnetic separation step to recover magnetic particles comprising steel from non-magnetic particles comprising copper, aluminium and plastic. Any suitable magnetic separation process or apparatus can be utilised, for example a high induction magnetic separator.

[0144] The steel particles may be sold as a product, or optionally recycled to be mixed with the lithium-ion battery feed (prior to step a). Alternatively, the steel particles may be added to the washing and attritioning step to assist with liberating electrode material. The non-magnetic particles comprising copper, aluminium and plastic may be collected for further processing or sale as a product. In some embodiments, the non-magnetic particles comprising copper, aluminium and plastic undergo further size reduction and classification or separation to recover copper and aluminium from the plastic particles, for example by using screens or screw classifier or wet gravity table, jig or up current classifier. Separated copper and aluminium may be dewatered and dried for sale.

[0145] The copper and aluminium depleted particles may undergo further classification and dewatering to separate plastic materials and electrode materials. Electrode material is separated and recycled to washing for recovery. Any aqueous liquid stream recovered from the dewatering stage is optionally recycled for use upstream in one or more shredding, washing, separation and attritioning steps as described herein.

Electrode material

[0146] In some embodiments, the separated particles comprising the electrode material at step b) are recovered as a wet filter cake.

[0147] In some embodiments, the filter cake comprises a water content in an amount of at least about 5, 10, 15, 20, 25, 30, 35, 40, 45 or 50% w/w based on the total weight of the filter cake. In some embodiments, the filter cake comprises a water content in an amount of less than about 50, 45, 40, 35, 30, 25, 20, 15, 10 or 5% w/w based on the total weight of the filter cake. Combinations of these values are also possible, for example between about 15% w/w to about 35% w/w. Alternatively, the wet filter cake is dried to remove some of the water content. The wet filter cake may be dried by any suitable means, for example in a flash, fluid bed or rotary drier or oven. The dried filter cake may comprise a water content in the amount of less than about 20, 15, 10, 8, 6, 4, 2, 1 or 0.1% w/w based on the total weight of the filter cake.

[0148] The separated particles at step b) comprise the electrode material. In some embodiments, at least one electrode material is selected from a cathode material or an anode material. In one embodiment, the separated particles at step b) comprise at least one electrode material. One or more impurities may also be present in the separated particles, for example one or more of copper, aluminium, plastic and steel. These impurities may be present in an amount of less than about 10, 9, 8, 7, 6, 5, 4, 3, 2, 1, 0.1, 0.01 or 0.001% w/w based on total weight of the separated particles.

[0149] In one embodiment, the separated particles at step b) comprise an anode material. In one embodiment, the separated particles comprise a cathode material. In one embodiment, the separated particles may each independently comprise a cathode material, an anode material, or a mixture thereof.

[0150] In some embodiments, the separated particles at step b) comprise a mixed metal material. It will be appreciated that the mixed metal material comprises at least cobalt and nickel values. In one embodiment, the mixed metal material may be a mixed metal oxide dust (MMD). In some embodiments, the MMD may be obtained during the recycling of lithium-ion batteries. The MMD may be a blend of one or more cathode materials obtained from lithium-ion batteries. In some embodiments, the MMD comprises lithium nickel manganese cobalt oxide (NMC), lithium cobalt oxide (LCO) or lithium nickel cobalt aluminium oxide (NCA), lithium manganese oxide (LMO), lithium ferro phosphate (LFP), lithium titanate (LTO) or a mixture thereof.

[0151] In some embodiments, the mixed metal material comprises cobalt, nickel and graphite.

[0152] In some embodiments, the mixed metal material may comprise at least about 1, 2, 5, 10, 15, 20, 25, 30, 35, 40, 45, 50 or 60% w/w cobalt. In some embodiments, the mixed metal material comprises less than about 60, 50, 45, 40, 35, 30, 25, 20, 15 or 10, 5, 2 or 1% w/w cobalt. Combinations of these % w/w values are also possible, for example the mixed metal material may comprise between about 2% w/w to between about 40% w/w cobalt, for example between about 5% w/w to about 30% w/w cobalt.

[0153] In some embodiments, the mixed metal material may comprise at least about 1, 2, 3, 4, 5, 6, 7, 8, 10, 15, 20, 30 or 40% w/w nickel. In some embodiments, the mixed metal material may comprises less than about 40, 30, 20, 15, 10, 8, 7, 6, 5, 4, 3, 2 or 1% w/w nickel. Combinations of these % w/w values are also possible, for example the mixed metal material may comprise between about 1% w/w to between about 20% w/w nickel, for example between about 2% w/w to about 15% w/w nickel. In some embodiments, the mixed metal material comprises between about 5% w/w to about 30% w/w cobalt and between about 2% w/w to about 15% w/w nickel.

[0154] One or more additional metal or non-metal values other than cobalt and nickel may be present in the mixed metal material in less than about 15, 10, 9, 8, 7, 6, 5, 4, 3, 2, 1, 0.1, 0.01 or 0.001% w/w based on total weight of the material. The additional metals may be selected from one or more of aluminium, graphite, arsenic, calcium, cadmium, chromium, copper, iron, potassium, lithium, magnesium, manganese, sodium, phosphorous, sulfur, silicon, zinc or fluorine.

[0155] The mixed metal material (e.g. MMD) may comprise one or more particulates (e.g. particles). The term “particle” (also referred to as “particulate”) refers to the form of discrete solid units. The units may take the form of flakes, fibres, agglomerates, granules, powders, spheres, pulverized materials or the like, as well as combinations thereof. The particles may have any desired shape including, but not limited to, cubic, rod like, polyhedral, spherical or semi-spherical, rounded or semi-rounded, angular, irregular, and so forth. In some embodiments, the mixed metal material may have an particle size. The particle size is taken to be the cross-sectional diameter across a particle. For non-spherical particles, the particle size is taken to be the distance corresponding to the longest cross-section dimension across the particle. In some embodiments, the mixed metal material comprises particles having a particle size of between about 1 pm to about 1,000 pm, about 1 pm to 500 pm, for example between about 5 pm to about 500 pm, e.g. between about 5 pm to about 200 pm, or between 10 pm to about 200 pm, or between 10 pm to about 50 pm.

[0156] The mixed metal material may have a particle size distribution (PSD), wherein 90% of the particles (P90) have a particle size of less than about 1000, 800, 500, 400, 300, 200, 120 or 100 pm, wherein 80% of the particles (Pso) have a particle size of less than about 800, 500, 400, 300, 200, 100 or 60 pm, wherein 50% of the particles (P50) have a particle size of less than about 500, 400, 300, 200, 100, 50 or 25 pm, wherein 20% of the particles (P20) have a particle size of less than about 200, 100, 50, 25, or 10 pm, or wherein 10% of the particles (P20) have a particle size of less than about 100, 80, 60, 40, 20, 10 or 5 pm. The particle size and/or PSD can be measured by any conventional method, including laser diffraction, electron microscopy, dynamic light scattering, optical microscopy or size exclusion methods (such as graduated mesh filters or screens).

Treatment of the dissolved or suspended electrolyte

[0157] During a typical lithium-ion battery recycling processes, recovered electrolyte compounds liberated during conventional shredding and dismantling are incinerated. In contrast, the present disclosure also provides a process to recover one or more electrolyte values from the dissolved or suspended electrolyte.

[0158] In one embodiment, at least part of the first and/or second aqueous liquid stream comprising dissolved or suspended electrolyte is further treated to remove (i.e. recover) one or more inorganic and organic species present in the first aqueous liquid stream.

[0159] Embodiments and examples provided above for the shredding process, aqueous slurry streams, aqueous liquid streams, aqueous input streams, and screening processes described herein in relation to obtaining an electrode material equally apply to the shredding and processing of lithium-ion batteries in relation to obtaining one or more electrolyte values described herein.

[0160] Although the recovery of captured electrolyte values is described in relation to the first and/or second aqueous liquid stream, it will be appreciated that such recovery can occur at any stage in the process where an aqueous liquid stream comprising dissolved or suspended electrolyte is generated. Fluoride recovery

[0161] One of the components of the electrolyte dissolved or suspended in the one or more liquid aqueous streams is fluoride, owing to the presence of LiPFe. In some embodiments, the first and/or second aqueous liquid stream comprising dissolved or suspended electrolyte is treated to remove and recover fluoride.

[0162] In one embodiment, lime is added to the first and/or second aqueous liquid stream to produce a fluoride precipitate. The lime may be hydrated lime (Ca(OH)2). In some embodiments, the lime is added to the first and/or second aqueous liquid stream in a stoichiometric excess based on the amount of fluorine in the first and/or second aqueous liquid stream. In some embodiments, the lime is added to the first and/or second aqueous liquid stream at a concentration of at least about 1, 5, 7, 10, 15, 20, 25, 30, 35 or 40 g/L (dry lime (CaO) basis) based on the volume of the aqueous liquid stream. In some embodiments, the lime is added to the first and/or second aqueous liquid stream at a concentration of less than about 40, 35, 30, 25, 20, 15, 10, 7, 5 or 1 g/L (dry lime (CaO) basis) based on the volume of the aqueous liquid stream. Combinations of these values are also possible, for example between about 2 g/L to about 30 g/L, or about 5 g/L to about 15 g/L.

[0163] The lime is mixed with the first and/or second aqueous liquid stream for a period of time effective to precipitate out fluoride from the aqueous liquid stream. In some embodiments, the fluoride precipitation may be performed for at least about 0.5, 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 12, 15, 20 or 24 hours. In some embodiments, the fluoride precipitation step may be performed for less than about 24, 20, 15, 12, 10, 9, 8, 7, 6, 5, 4, 3, 2, 1 or 0.5 hours. Combinations of these residence times are also possible, for example between about 1 hour to about 8 hours, or about 2 hours to 6 hours.

[0164] The fluoride precipitation step may be performed at a suitable temperature. In some embodiments, the fluoride precipitation step may performed at a temperature of at least about 5, 10, 15, 20, 25, 30, 35, 40, 45, 50, 55 or 60°C. In other embodiments, the fluoride precipitation step may be performed at a temperature of less than about 60, 55, 50, 45, 40, 35, 30, 25, 20, 15, 10 or 5°C. Combinations of these values are also possible, for example between about 10°C to about 50°C, or about 25 °C to about 35 °C. The temperature of the precipitation step may be controlled by any suitable means, for example a heat exchanger or immersed coils.

[0165] In some embodiments, the fluoride is recovered from the first and/or second aqueous liquid stream as a calcium fluoride or calcium fluoroapatite or a combination thereof. Possible precipitation reaction are provided as follows:

(1) 2LiF(aq) + Ca(OH)₂(aq) = CaF₂(s) + 2LiOH(aq)

(2) 5Ca(OH)₂(aq) + 3LiH₂PO₄/Li₂HPO₄ (aq) + NaF(a) = Ca₅(PO₄)₃F (s)+ 3LiOH(a) + NaOH(a) + 6H₂O(1)

[0166] In some embodiments, the fluoride precipitate is separated from the first and/or second aqueous liquid stream to produce a fluoride depleted liquor. Suitable separation techniques include, but are not limited to, filtration, gravity separation, centrifugation, decantation and so forth.

Lithium recovery

[0167] Another main component of the electrolyte dissolved or suspended in the one or more liquid aqueous streams is lithium. In some embodiments, the fluoride depleted liquor comprises dissolved lithium. In some embodiments, the fluoride depleted liquor may be treated to recover lithium.

[0168] In some embodiments, the fluoride depleted liquor is treated to produce a lithium phosphate precipitate. The lithium phosphate precipitate may be recovered by adding a source of phosphate to the fluoride depleted liquor. In some embodiments, lithium is recovered from the fluoride depleted liquor by: a) adding phosphate to the fluoride depleted liquor to produce a lithium phosphate precipitate; and b) separating the lithium phosphate precipitate from the liquor solution produced in step a) defined above in relation to this embodiment.

[0169] The phosphate may be selected from the group comprising phosphoric acid, potassium phosphate, sodium phosphate, or a combination thereof.

[0170] In some embodiments, phosphate is added to the fluoride depleted liquor in step a) in stoichiometric excess based on the amount of lithium in the liquor. In some embodiments phosphate is added to the liquor in an amount of at least about 0.1, 0.5, 1, 5, 10, 20, 30, 40 or 50 gram of phosphate per gram of lithium in the liquor. In some embodiments phosphate is added to the liquor in an amount less than about 50, 40, 30, 20, 10, 5, 1, 0.5 or 0.1 gram of phosphate per gram of lithium in the liquor.

Combinations of these g/g values are also possible, for example between about 1 g/g to about 50 g/g.

[0171] In some embodiments, the lithium phosphate precipitation step may be performed at a temperature of at least about 40, 50, 60, 70, 80, 90, 95 or 100°C. In some embodiments, the lithium phosphate precipitation step may be performed at a temperature of less than about 100, 95, 90, 80, 70, 60, 50 or 40°C. Combinations of these values are also possible, for example between about 50°C to about 100°C, or about 75 °C to up to the boiling point of the liquor.

[0172] Lithium is expected to be recovered as a lithium phosphate (Li₃PO₄), as shown in the reactions below:

(1) 3Li₂CO₃(aq) + 2Na₃PO₄(aq) = 2Li₃PO₄(s)+ 3Na₂CO₃(aq)

(2) 6Li₂HPO₄/ LiH₂PO₄ (aq) + 3Ca(OH)₂(aq) = 4Li₃PO₄(s) + Ca₃(PO4)₂(s) + 6H₂O(1)

[0173] In some embodiments, lime may also be added with the phosphate. The addition of lime may assist with the conversion of the lithium hydrogen phosphate species to generate the lithium phosphate and/or reduce the final phosphate concentration in the solution.

[0174] The lithium phosphate precipitate may be separated from the liquor by conventional separation techniques and washed in several stages. Suitable separation techniques include, but are not limited to, filtration, gravity separation, centrifugation, decantation and so forth. Separating the lithium phosphate produces a fluoride and lithium depleted liquor (also referred to as the depleted liquor).

[0175] The separated lithium phosphate precipitate may then be optionally dried and transported for sale or disposal. Alternatively, or additionally, in some embodiments the lithium phosphate precipitate may then be treated to re-precipitate lithium phosphate, thereby reducing the presence of impurities

[0176] In some embodiments, the lithium phosphate precipitate may be mixed with phosphoric acid to produce a slurry having % solids in the range of 15% to 50% w/w, for example of 35% to 45% w/w. The amount of phosphoric acid required may be sub- stoichiometric with respect to the complete “dissolution” of the lithium phosphate precipitate as Li2HPO4. For example, the amount of phosphoric acid required may be in the range of 50 kg/t to 250 kg/t of lithium phosphate precipitate.

[0177] The step of re-precipitating lithium phosphate may be performed at ambient temperature or around 30°C. The dissolution and re-precipitation of lithium phosphate may be performed for a period of between 4 hours to 24 hours. A residence time of about 24 hours may be beneficial to achieve the maximum rejection of impurities at lower stoichiometric additions of phosphoric acid.

[0178] Recovery of lithium as re-precipitated lithium phosphate may be greater than 95%. It will be appreciated that the amount of lithium phosphate remaining soluble in the liquor from the refining step may be dependent on the pH and solids content of the process stream. In one embodiment, the pH may be in a range of pH 4 to pH 6.5, in particular pH 5 to pH 6, for example about pH 5, 5.2, 5.4, 5.6, 5.8 or 6, and combinations thereof.

[0179] The re-precipitated lithium phosphate precipitate may be separated from solution by conventional separation techniques and washed in several stages. Suitable separation techniques include, but are not limited to, filtration, gravity separation, centrifugation, decantation and so forth. Potassium hydroxide may be subsequently added to the separated liquor to regenerate a potassium phosphate stream. At least part of the potassium phosphate stream may then be recycled as the source of phosphate.

[0180] In some embodiments, lithium phosphate may be recovered using the process described in PCT/AU/2019/050540, the contents of which are incorporated herein by reference.

[0181] It will be appreciated that while the lithium recovery described above is in relation to a fluoride depleted liquor, it will be appreciated that lithium could be recovered from aqueous liquid streams comprising fluoride. For example, the fluoride recovery and lithium recovery steps can be performed in any order prior to the recovery of organic electrolytes (see below) as understood by the person skilled in the art.

Organic electrolytes

[0182] In some embodiments, the depleted liquor is further treated to remove one or more other organic compounds (e.g. organic phases) by oxidation to produce a treated third aqueous liquid stream.

[0183] Organic electrolyte compounds present in the depleted liquor may include ethylene glycol, alkyl carbonate (e.g. ethylene carbonate (EC), dimethyl carbonate (DEC), propylene carbonate (PC), ethylene methyl carbonate (EMC), fluoroethylene carbonate (FC), vinylene carbonate (VC)), 1,3-propane sulfone, 2-propynyl methanesulfonate, cyclohexylbenzene. [0184] In one embodiment, the depleted liquor is treated with an oxidising agent to remove the organic electrolyte. In one embodiment, the depleted liquor is treated with hydrogen peroxide to remove ethylene glycol, as shown in the reaction below:

(1) 2H₂O₂(1) = 2H₂O(1) + O₂(g)

(2) 2C₂H₆O₂(aq) + 5O₂(g) = 4CO₂(g) + 6H₂O(1)

[0185] In one embodiment, organic compounds can be removed by introduction of a biological enzyme specifically targeted for the organic compounds present.

[0186] In one embodiment, organic compounds can be selectively recovered by fractional distillation or membrane electrolysis.

[0187] In some embodiments, the treated third aqueous liquid stream is recycled for use in one or more shredding, washing, separation and attritioning steps as described herein.

[0188] The present application claims priority from AU2020902848 filed on 12 August 2020, the entire contents of which are incorporated herein by reference.

EXAMPLES

[0189] In order that the disclosure may be more clearly understood, particular embodiments of the invention are described in further detail below by reference to the following non-limiting experimental materials, methodologies and examples.

Example 1: Embodiment of process for recovering values from lithium-ion batteries.

[0190] Referring to Figure 1, sorted lithium-ion batteries 100, are initially shredded 104 using a twin shaft shredder in the presence of a continuous aqueous input stream 150 to produce a first aqueous slurry comprising shredded battery particles 139. The shredded lithium-ion batteries 139 undergo a separation step 224 to obtain the electrode material 230, and a first aqueous liquid stream 120. Aqueous make-up (e.g. water) 145 is added as required to the aqueous input stream 150, or directly to the shredding 104. Off-gas treatment 600, is provided to contain any fugitive emissions during the shredding step 104.

[0191] At least part of the first aqueous liquid stream 120 is recycled to the aqueous input stream 150. At least part of the first aqueous liquid stream 120 is treated to remove one or more electrolyte values. For example, one or more fluoride, lithium and phosphate 554 can be recovered by treating the first aqueous liquid stream 500.

[0192] For example, referring to Figure 1, at least part of the first aqueous liquid stream 120 is reacted 500, with hydrated lime 501 and sodium phosphate 502, to precipitate fluoride and lithium. The fluoride and lithium precipitate is recovered as a filter cake 554. Liquor depleted in fluoride, lithium and phosphate undergoes further processing to remove miscible organic compounds by oxidation, for example ethylene glycol.

[0193] Treated aqueous stream 570, depleted in fluoride, phosphate, lithium and miscible organic compounds is available for recycling and re-use in the process.

[0194] Referring to Figure 2, sorted lithium-ion batteries 100, are intially shredded 105 using a twin shaft shredder in the presence of a continuous aqueous input stream 150 to produce a first aqueous slurry comprising shredded battery particles 110. The first aqueous slurry comprising shredded battery particles 110, undergoes classification and dewatering 115, using a device such as a screw classifier or screen and thickener to produce a second aqueous slurry stream comprising coarser shredded battery particles 130 and a third aqueous slurry stream comprising a portion of electrode material (e.g. mixed cathode and anode material) 125. The first aqueous liquid stream is recovered and recycled 120 and the third aqueous slurry stream 125 is added to shredded product washing and attritioning 200. Aqueous make-up (e.g. water) 145 is added as required to the aqueous input stream 150, or directly to the initial shredding 105 or classification and dewatering stage 115. Off-gas treatment 600, is provided to contain any fugitive emissions.

[0195] The second aqueous slurry comprising classified and dewatered coarser shredded battery particles 130 are subject to a second stage of shredding 135, using a single or twin shaft shredder without water to reduce the particle size, and are combining with the third aqueous slurry stream 125 to obtain the first aqueous slurry stream comprising shredded battery particles 140.

[0196] The shredded lithium-ion battery particles 140 are washed and attritioned 200, using a device such as a washing drum or trommel and or an agitated attritioning cell, with aqueous wash solution addition as necessary 275. A slurry of washed shredded lithium-ion battery particles 205 undergoes size separation 210 using a screen or similar physical separation device. Screen oversize material 215 progresses to steel recovery and screen undersize material 220 undergoes solid liquid separation 225 to obtain the electrode material 230 and a second aqueous liquid stream 240. Aqueous make-up (e.g. water) 270 is added as required to aqueous wash solution 275, or directly to the product washing and attritioning 200 (not shown), size separation 210 (not shown) or solid liquid separation 225 (not shown) stage. The second aqueous liquid stream 240 is treated to recover one or more electrolyte compounds (see 504, 530 and 565).

[0197] The electrode material (e.g. mixed cathode and anode material) 230 is available for sale as a solid filter cake product. Recovered aqueous solution is either recycled 235 for product washing and attritioning 200, optionally recycled for use in the continuous aqueous input stream 240, or further treated 240 to remove captured electrolyte components.

[0198] Steel is recovered by magnetic separation 300, with the separated steel product 305 collected for sale or optionally recycled 310. Non-magnetic material 315, is collected for further processing or sale as a product. [0199] Referring to Figure 2, fluoride contained in the second aqueous liquid stream 240 is reacted 504 with hydrated lime 505, with the dilute slurry 510 undergoing solid liquid separation and washing 515. The fluoride precipitate is recovered as a filter cake 520, with fluoride depleted liquor 525 undergoing processing 530 with lime 535 and sodium phosphate 540 to recover lithium as lithium phosphate (LisPC ). The dilute slurry 545 undergoes solid liquid separation 550, with the lithium phosphate precipitate separated and washed. A lithium phosphate precipitate is recovered as a filter cake 555. Liquor depleted in fluoride, lithium and phosphate 560 undergoes further processing 565 to remove miscible organic compounds by oxidation, for example ethylene glycol.

Example 2: Embodiment of process incorporation of wet copper, aluminium and plastic separation

[0200] Referring to Figure 3, non-magnetic material, including copper, aluminium and plastic 315 undergoes size reduction and water based gravity separation 400, using devices such as screw classifiers, wet gravity tables, up current classifiers or dense media separation. Separated copper 405 and aluminium 410 products are dewatered and dried for sale.

[0201] Plastic 415 undergoes further classification and dewatered 420, using devices such as spiral or up-current classifiers, to generate a recovered plastic product 425, an electrode material product and an aqueous stream, that can be optionally combined for recycle 430 or sent to solid liquid separation 435.

Example 3: Embodiment of process incorporation of dry copper, aluminium and plastic separation

[0202] Referring to Figure 4, non-magnetic material, including copper, aluminium and plastic 315 undergoes size reduction and dry based size separation 401, using devices such as screens and or air classifiers. Separated coarse plastic 440, mixed copper and aluminium 445 and mixed fine plastic and electrode material 450 are recovered as products. [0203] Fine plastic and electrode material can be optionally recycled to the washing and attritioning stage 200 and combined with the first aqueous slurry stream.

Example 4: Embodiment of process incorporating separation of the cathode and anode material

[0204] Referring to Figure 5, screen undersize electrode material (e.g. mixed cathode and anode material) 220 undergoes gravity separation 245, using a device such as gravity spirals, jig, up current classifier, dense media separation or a high-g gravity separator such as a Knelson concentrator, centrifuge or multi gravity separator. Cathode material recovered as a heavy concentrate is separated and dewatered and optionally dried as a product 250 for sale.

[0205] Anode material reports to the light gravity product 255 and undergoes solid liquid separation 260 to recover anode material as a solid filter cake product 265 and optionally dried for sale as a product. Recovered aqueous solution is either recycled 235 for product washing and attritioning 200, optionally recycled for use in the continuous aqueous input stream 240, or further treated 240 to remove captured electrolyte components.

Example 5: Obtaining of electrode material and liberation of electrolyte compounds from lithium-ion batteries

[0206] 5 tonnes of spent lithium-ion batteries were shredded in multiple stages and washed as a production run. Recovered products included, 1.8 tonnes of mixed cathode and anode material as a wet filter cake, 0.9 tonne as steel and 3.5 tonnes as mixed copper, aluminium and plastic, with all product masses including the presence of process water.

[0207] The elemental composition of the mixed cathode and anode material obtained using the process described herein is summarised in Table 1 : Table 1: Composition of mixed cathode and anode material liberated and recovered via the process described herein.

[0208] Staged liberation of electrolyte compounds and progressive capture of electrolyte compounds into process water, during the shredding of the 5 tonnes of spent lithium-ion batteries, is shown in Table 2. [0209] Electrolyte compounds progressively accumulate as process water and is recycled and re-used in the process, maintaining the pH over 8, which is important to mitigate against aqueous HF formation.

Table 2: Progressive capture of electrolyte components

Example 5: Fluoride removal from aqueous liquid streams

[0210] A sample of process water was reacted with lime at ambient temperature.

Hydrated lime (Ca(OH)2) was added on a stoichiometric excess basis.

[0211] Fluoride can be precipitated in 4 hours on batch basis at 30°C, to levels below 20 mg/L, selective to lithium, as shown in Table 3.

Table 3: Selective removal of fluoride

[0212] By increasing temperature and adding a stoichiometric excess of sodium phosphate (NasPCb) lithium can be partially precipitated in conjunction with fluoride. [0213] Table 4 shows reaction of proves water with stoichiometric excess sodium phosphate and hydrated lime at 95 °C, for 4 hours. Lithium is reduced to below 250 mg/L in 2 hours.

Table 4: Removal of lithium

Example 6: Optimised recovering of electrode material

[0214] A sample of mixed cathode and anode powder was wet screened at 150 pm and the plus 150 pm fraction processed in attritioning cell at 50% w/w.

[0215] Table 5 shows the impact of attritioning scrubbing in terms of liberating cathode and anode powder adhered to the surface of copper and aluminium, generating additional minus 150 pm material, which is lower in copper and aluminium and higher in cobalt than the feed material.

Table 5: Impacts of attrition scrubbing on mixed cathode and anode material Example 7: Separating anode material and cathode material

[0216] A sample of mixed cathode and anode powder was subject to a single stage of gravity separation. Three product streams were generated with cathode material (metal oxides) concentrating in heavy fraction and anode material (carbon) in the light fraction, as shown in Table 6. Multiple stages of gravity separation would be expected to provide improved separation and recovery of cathode material to the heavy fraction and anode material to the light fraction.

Table 6: Gravity concentration of cathode material

[0210] It will be appreciated by persons skilled in the art that numerous variations and/or modifications may be made to the above-described embodiments, without departing from the broad general scope of the present disclosure. The present embodiments are, therefore, to be considered in all respects as illustrative and not restrictive.

Claims

58 CLAIMS:

1. A process for obtaining an electrode material from lithium-ion batteries, the process comprising the steps of: a) shredding lithium-ion batteries in the presence of a continuous aqueous input stream to obtain a first aqueous slurry stream comprising an aqueous phase, shredded battery particles and an electrolyte, wherein the particles comprise coarser particles of copper, aluminium, plastic and steel and finer particles of electrode material, and the electrolyte is dissolved or suspended in the aqueous phase of the first aqueous slurry stream; b) separating and obtaining coarser particles of copper, aluminium, plastic and steel and finer particles of electrode material from the first aqueous slurry stream and producing a first aqueous liquid stream comprising dissolved or suspended electrolyte; and c) recycling at least part of the first aqueous liquid stream comprising dissolved or suspended electrolyte to the shredding at step a) for use in the continuous aqueous input stream.

2. The process of claim 1, wherein the separating and obtaining the coarser and finer particles at step b) comprises: bl) dewatering and classifying the first aqueous slurry stream comprising the shredded battery particles based on particle size to produce a second aqueous slurry stream comprising the coarser particles, a third aqueous slurry stream comprising the finer particles, and the first aqueous liquid stream; b2) subjecting the second aqueous slurry stream comprising the coarser particles to further shredding to obtain a size-reduced second aqueous slurry stream; b3) combining the size-reduced second aqueous slurry stream with the third aqueous slurry stream to obtain the first aqueous slurry stream and separating the particles therefrom and producing a second aqueous liquid stream comprising dissolved or suspended electrolyte and optionally recycling at least part of the second aqueous liquid stream comprising dissolved or suspended electrolyte to the shredding at step a) for use in the continuous aqueous input stream. 59

3. The process of claim 2, wherein the further shredding of the second aqueous slurry stream reduces the average particle size of the coarser particles therein, wherein 90% of the particles (P90) have a particle size of less than about 10,000 pm.

4. The process of claim 2 or claim 3, wherein the further shredding of the size reduced second aqueous slurry stream is performed in the presence of a second continuous aqueous input stream.

5. The process of any one of claims 2 to 4, wherein the second aqueous slurry stream has a solids concentration of between 60% w/w to 99% w/w based on the total weight of the second aqueous slurry stream.

6. The process of any one of claims 2 to 5, wherein the third aqueous slurry stream has a solids concentration of between 5% w/w to 50% w/w based on the total weight of the third aqueous slurry stream.

7. The process of any one of claims 2 to 6, wherein the third aqueous slurry stream comprises finer particles having an average particle size of less than about 500 pm.

8. The process of any one of claims 2 to 7, wherein third aqueous slurry stream comprises between about 1% to about 30% of the total electrode material present in the first aqueous slurry stream.

9. The process of any one of claims 1 to 8, wherein the first and/or second aqueous liquid stream has a solids concentration of less than about 5% w/w based on the total weight of the aqueous stream.

10. The process of any one of claims 2 to 9, further comprising washing and/or attritioning the first aqueous slurry stream comprising the coarser particles of copper, 60 aluminium, plastic and steel and finer particles of electrode material with an aqueous wash solution prior to separating the particles therefrom at step b).

11. The process of claim 10, wherein the amount of aqueous wash solution added during the washing step provides the first aqueous slurry stream with a solids concentration of between about 5% w/w to about 70% w/w based on the total weight of the first aqueous slurry stream.

12. The process of any one of claims 1 to 11, wherein the separating and obtaining the coarser and finer particles at step b) comprises a wet-size separation step to remove coarser particles comprising copper, aluminium, plastic and steel from the first aqueous slurry stream to produce a separated first aqueous slurry stream comprising finer particles wherein the finer particles comprise the electrode material.

13. The process of claim 12, wherein the wet-size separation is completed at about 1,000 pm or less.

14. The process of claim 12 or claim 13, wherein the separated coarser particles comprising copper, aluminium, plastic and steel is subjected to a magnetic separation step to recover magnetic particles comprising steel which is optionally recycled into the lithium-ion battery feed at step a), and non-magnetic particles comprising copper, aluminium and plastic.

15. The process of claim 14, wherein the non-magnetic particles comprising copper, aluminium and plastic undergo gravity separation to separate copper and aluminium from the plastic particles.

16. The process of any one of claims 1 to 15, wherein the separated particles comprising the electrode material at step b) are recovered as a wet filter cake. 61

17. The process of claim 16, wherein the filter cake comprises a water content in an amount of between about 10% w/w to about 40% w/w based on the total weight of the filter cake.

18. The process of claim 16 or claim 17, wherein the wet filter cake is dried to remove some of the water content.

19. The process of any one of claims 1 to 18, wherein at least one electrode material is selected from a cathode material and an anode material.

20. The process of claim 19, wherein the cathode material comprises a mixed metal material.

21. The process of claim 20, wherein the mixed metal material comprises cobalt nickel and graphite.

22. The process of claim 21, wherein the mixed metal material comprises lithium nickel manganese cobalt oxide (NMC), lithium cobalt oxide (LCO) or lithium nickel cobalt aluminium oxide (NCA), lithium manganese oxide (LMO), lithium ferro phosphate (LFP) lithium titanate (LTO) or a mixture thereof.

23. The process of any one of claims 19 to 22, wherein following step b) the separated particles comprising the electrode material undergo gravity separation to separate the cathode material from the anode material.

24. The process of any one of claims 1 to 23, wherein the recycling of the first aqueous stream comprising dissolved or suspended electrolyte is provided to maintain the pH of the continuous aqueous input stream between about pH 6 to about pH 12.

25. The process of any one of claims 1 to 24, wherein the electrolyte dissolved or suspended in the first and/or second aqueous liquid stream comprises one or more of 62 lithium hexafluorophosphate (LiPFe), an alkyl carbonate (e.g. ethylene carbonate (EC), dimethyl carbonate (DEC), propylene carbonate (PC), ethylene methyl carbonate (EMC), fluoroethylene carbonate (FC), vinylene carbonate (VC)) 1,3-propane sulfone, 2-propynyl methanesulfonate, cyclohexylbenzene, imidazolium cations, and pyrrolidinium anions.

26. The process of claim 25, wherein the concentration of lithium in the first and/or second aqueous liquid stream comprising dissolved or suspended electrolyte is between about 200 mg/L to about 10,000 mg/L based on the volume of the aqueous liquid stream.

27. The process of claim 25 or claim 26, wherein the concentration of fluoride in the first and/or second aqueous liquid stream comprising dissolved or suspended electrolyte is between about 100 mg/L to about 1,000 mg/L based on the volume of the aqueous liquid stream.

28. The process of any one of claims 26 to 27, wherein the concentration of phosphorous in the first and/or second aqueous liquid stream comprising dissolved or suspended electrolyte is between about 200 mg/L to about 5,000 mg/L based on the volume of the aqueous liquid stream.

29. The process of any one of claims 1 to 28, wherein the continuous aqueous input stream has a flow rate of between about 0.1 nr'/tonne to about 100 m³/tonne of aqueous input stream per tonne of lithium-ion battery.

30. The process of any one of claims 1 to 29, wherein the first and/or second aqueous liquid stream comprising dissolved or suspended electrolyte is further treated to remove one or more inorganic and organic species present in the first and/or second aqueous liquid stream.

31. The process of claim 30, wherein lime is added to the first and/or second aqueous liquid stream to produce a fluoride precipitate.

32. The process of claim 31, wherein the fluoride precipitate comprises calcium fluoride or calcium fluoroapatite or a combination thereof.

33. The process of claim 31 or claim 32, wherein the lime is added to the first and/or second aqueous liquid stream in a stoichiometric excess based on the amount of fluorine in the first aqueous liquid electrolyte stream based on the volume of process water in the first and/or second aqueous liquid stream.

34. The process of any one of claims 31 to 33, wherein fluoride precipitation reaction is performed at a temperature of less than about 50°C.

35. The process of any one of claims 31 to 34, wherein the fluoride precipitation reaction is performed for a period of time of between about 1 hour to about 10 hours.

36. The process of any one of claims 31 to 35, wherein the fluoride precipitate is separated from the first and/or second aqueous liquid stream to produce a fluoride depleted liquor.

37. The process of claim 36, wherein lithium is recovered from the fluoride depleted liquor by adding a source of phosphate and optionally lime to produce a lithium phosphate precipitate.

38. The process of claim 37, wherein the source of phosphate is phosphoric acid, potassium phosphate, sodium phosphate or combinations thereof, preferably sodium phosphate.

39. The process of claim 37 or claim 38, wherein the source of phosphate is added to the fluoride depleted liquor in stoichiometric excess based on the amount of lithium in the fluoride depleted liquor.

40. The process of any one of claims 37 to 39, wherein the lithium precipitation reaction is performed at a temperature of greater than 50°C, or between about 75°C up to the boiling point of the fluoride depleted liquor.

41. The process of any one of claims 37 to 40, wherein the lithium phosphate precipitate is separated from the fluoride depleted liquor to produce a fluorine and lithium depleted liquor.

42. The process of claim 41, wherein the depleted liquor is further treated to remove one or more other organic compounds by oxidation to produce a treated third aqueous liquid stream.

43. The process of claim 42, wherein the treated third aqueous liquid stream is recycled for use in one or more shredding, washing and attritioning and separation steps as defined in any one or more of the preceding claims.