Lithium ion battery recycling method

Abstract

The present invention relates to an efficient and environmentally friendly recycling method of lithium ion batteries, which includes detaching the lithium ion batteries to obtain lithium ion battery cell components, such as cathodes, with high amounts and high quality of corresponding active material compositions for further material recovery in hydrometallurgical processes.

Description

Technical Field

[0001] The present invention relates to the recycling of lithium-ion batteries; in particular in electric transportation applications like but not limited to electric vehicles, a highly efficient recycling method for lithium-ion batteries is provided, which obtains high recovery rates through effective pretreatment and hydrometallurgical procedures. Background Art

[0002] Currently, lithium-ion batteries (LiB) are considered to be a particularly reliable and efficient technology for sustainable and green (electric) energy storage systems due to several reasons such as high energy density and power per unit battery weight, allowing them to be lighter and smaller than other rechargeable batteries. New research and manufacturing methods for lithium-ion batteries are providing increased storage capacity, faster charging speeds and longer overall lifespan. However, new developments and innovations in this field are strongly dependent on the availability and price of raw materials mined in non-European and non-Mediterranean countries and mainly by foreign entities. In addition, the raw materials required for the manufacture of new lithium-ion batteries are of limited availability due to limited and low reserves; thus, the risk of depletion and demand outweighing supply has been real so far (for example, in the case of cobalt, lithium and nickel).

[0003] In addition, from the perspective of sustainability, raw materials such as cobalt (Co), nickel (Ni), manganese (Mn) and lithium (Li) are extracted from natural minerals that require mining operations in large areas (even farmland or residential areas in some cases) and use chemical hazardous treatments. These extraction operations strongly cause the environment and air to be polluted by heavy metals and consume a large amount of water. In addition, the use of high-throughput machines for extraction and treatment leads to the emission of greenhouse gases. Therefore, with the growth of global demand for lithium-ion battery manufacturing, environmentally sustainable and economically viable recycling technologies are becoming key focus areas. Therefore, alternative material sources for lithium-ion batteries are paid attention to and valued in modern society, and recycling is thus a major technology related in this case.

[0004] Prior art lithium-ion battery recycling considers the recycling of lithium-ion battery cathode active materials, such as lithium-nickel-manganese-cobalt-oxide (NMC), lithium-cobalt-oxide (LCO), lithium-manganese-oxide (LMO) or lithium-nickel-oxide (LNO) compositions, while other important components of lithium-ion batteries are either not considered, poorly recycled or destroyed. Recycling and recovery are mainly focused on winning cathode active materials due to the economic overload weight of cathode materials. Recycling of lithium battery materials can be carried out by recovering cathode material compositions as a combination of products and compounds with different stoichiometric cathode active elements nickel, cobalt, manganese and lithium. This powder mixture of active material compounds with different chemical element contents is an agglomerate, usually called "black mass", in which impurities of iron, phosphorus, aluminum, copper and plastics may still be present. It is important to emphasize that the initial cathode active materials, such as nickel-manganese-cobalt, lithium-cobalt-oxide or lithium-iron-phosphate (LFP) are not recycled and recovered as individual chemically pure elements, but as aggregate chemical products / compounds with a certain degree of impurities as precursor materials. When the input material mass is considered as the output material mass (input mass relative to the recovered mass of the output material), some recycling programs recover elements, but can only achieve recycling efficiencies below 80% (under optimistic assumptions). Anode materials and other implemented materials, such as metal collectors, are also recovered, however mainly in the form of mixed and crushed powders that are recovered with high impurity levels and require additional purification steps.

[0005] The core process of the current recycling method solves "shredding / crushing" as a mechanical pretreatment process in order to reduce the volume and obtain up to 75% of the mass of the active material realized in the lithium-ion battery by crushing the lithium-ion battery into small-sized pieces. To this end, the lithium-ion battery module (with housing, plastic, adhesive, connector, battery cell, etc.) is reduced by chopping it into micron particle size before separating the different materials of the received powder mixture into active materials such as cathode, anode and collector materials. In this process, the material is subjected to high stress, temperature and force, whereby some particles are incinerated, destroyed or irreversibly changed, making it impossible to recycle these materials. Most often, the mechanical pretreatment is not completed by utilizing a single crushing step but by at least 2 crushing treatment steps, and some recycling methods do not show improvements for the 3 crushing treatment steps also available in the industry. In addition, complex screening, cleaning and post-treatment processes are required to obtain a processable black substance after crushing.

[0006] Current recycling methods consider the following steps for recovering ferrous materials:

[0007] Shredding as a pre-treatment for leaching with mineral acids and highly complex separation treatments:

[0008] - Lithium-ion battery pack discharge

[0009] - Open the lithium-ion battery pack and separate the lithium-ion battery modules

[0010] - Shredding of entire lithium-ion battery modules (with metal, plastic, etc.)

[0011] -Magnetic separation / flotation / filtration / extraction of metal and plastic substances

[0012] - Clean the powder by leaching using mineral acids

[0013] - Extraction of black matter (e.g. NMC) or separation of materials with low reusability and recycling efficiency.

[0014] Dismantling as a pre-treatment for leaching with mineral acids without further separation of the elements:

[0015] - Lithium-ion battery pack discharge

[0016] - Open the lithium-ion battery pack and disassemble the lithium-ion battery module

[0017] -Open the lithium-ion module and disassemble it into lithium-ion battery cells

[0018] -Open the lithium-ion battery cell

[0019] -Washing lithium-ion cells in liquid to remove electrolyte

[0020] - Separation of cathode and anode (active material + collector foil)

[0021] - Leaching of cathode active material with high pressure mineral acid stream to separate active material from collector

[0022] - Cleaning active materials

[0023] - Extraction of black matter (such as NMC)

[0024] An example of such an application is disclosed in the published patent application CN108285977A. The application discloses a method for recycling waste lithium-ion battery positive electrode materials. The method comprises the following steps: discharging the lithium-ion battery, decomposing it, and crushing the lithium-ion battery to obtain a positive electrode sheet, leaching treatment, and drying treatment. In this method, the material is crushed, so that different metals need to be extracted before leaching, which increases the impurities of the material.

[0025] The disadvantages of obtaining recycling treatments of active materials as black matter and the processing steps they apply will be managed separately below:

[0026] Shredding: Due to mechanical procedures with high forces, pressures and stresses, the input material is crushed, ground and incinerated at local extremes. In addition, by applying an inert medium (to suppress discharges or other undesirable reactions in the shredding process), the shredding mechanism leads to the destruction and incineration of key raw materials, resulting in high material losses between 20% and 40%, with the resultant loss of valuable materials. As a result, the recycling efficiency of the system "batteries to materials" has only an efficiency of less than 80%. This means that, in terms of current raw material values, 1 ton of lithium-ion battery (NMC) input material involves an economic loss of up to 1'150 euros. In 2030, a conservative calculation of the available lithium-ion battery recycling material is up to 3'000'000 tons, which involves an economic loss of up to 3'450 million euros in terms of material value. Knowing that the raw materials (resources and reserves) for the manufacture of lithium-ion batteries are limited and that the demand for lithium-ion batteries is expected to grow exponentially in the coming years, the application of shredders is neither economically nor ecologically profitable or desirable in the long term. Furthermore, shredding of lithium-ion batteries is not a clean technology that provides a reusable product for the lithium-ion battery industry. The powder obtained by a single-step shredding is usually insufficient, so multi-step shredding is usually applied. In addition, the powder has a high impurity level, thereby requiring a variety of post-processing methods such as flotation, magnetic separation, multi-step screening, etc., which increases the number of processing steps, complexity, operating costs and reduces the final yield.

[0027] Disassembly and inorganic leaching to obtain black matter: In the prior art methods, the leaching step is combined with a separation step, in which the cathode active material is separated from the collector by applying a (high pressure) flow of inorganic acid. Although the procedure may take less time due to the combination of 2 processing steps in one step (separation and leaching of active material from the collector), more material is lost due to the strong impact and dispersion of the separated material dissolved in the liquid phase, and additional impurities are introduced due to the strong interaction with the metal collector, so that there is no effective material recovery. A cleaning / purification step is required after this leaching treatment (usually in the form of filtration or sieving), in which the dissolved cathode active material is collected and dried, thereby obtaining black matter, an accumulation / compound of active materials.

[0028] Low quality recycled material / final product or only precursor: Another major disadvantage of the shredding and separation into black mass or manual disassembly and separation into black mass procedure is that the final product or recycled material is a composition of different materials with unknown properties, purity, and a mixture of different chemical elements, products and compounds. Therefore, the properties of the final black mass are strongly dependent on the input cathode active material. Obtaining only black mass severely limits the usability of the output material because the chemical composition of the cathode active material has different ratios / stoichiometric compositions, such as N:M:C=1:1:1 or 8:1:1 or 5:3:2. This means that in the recovery / recycling process of the active material, disassembly or shredding of the input material to NMC level is only feasible when the same active material chemistry (ratio) is used to build a new cathode; thus also limiting the use of only one fixed input material chemistry. Therefore, an ideal recycling process using a battery input stream based on NMC 1:1:1 active material is able to produce a black mass close to the NMC 1:1:1 chemical composition, which can be used to manufacture lithium-ion batteries with a cathode active material chemical composition of NMC 1:1:1. However, this assumption is valid when, for example, input lithium-ion batteries - NMC are used, if the previous leaching treatment is tailored to maximize the leaching capacity of the cathode active material by recovering almost 100% of the input elements nickel, manganese, cobalt, lithium. Otherwise, the final ratios of the elements will vary and a final product with the desired chemical ratios cannot be ensured. In all other cases with mixed input materials, the final mixture of black mass with cathode active materials of various chemical substances can hardly or cannot be used for the manufacture of lithium-ion batteries. Moreover, the recovered black mass cannot be fully used to build new lithium-ion battery cells with a share of 100% recycled / recovered materials, but is limited to the current share of 10% combined with 90% of new virgin materials, which is generally not achievable assuming a high purity of the recycled materials.

[0029] Hazardous gases and wastewaters due to the use of inorganic acids in the leaching process: The use of inorganic leaching agents for the recovery of lithium-ion battery materials is a common factor in both processes leading to the generation and emission of hazardous gases and fluids dangerous to humans and nature, which are partly caused by the impure pre-treatment and its associated post-pre-treatment to obtain the black material. In addition, this increases the pollution of the environment by hazardous reagents, which may also cause poisoning of workers. In addition to this, the use of hazardous reagents requires high active and passive safety and health standards for operators and workers, which are difficult to meet in recycling facilities. Summary of the invention

[0030] The present invention solves the following problems and challenges of current prior art solutions for recycling lithium-ion batteries (for those given in the prior art section and other solutions not mentioned above):

[0031] - High waiting / dead time due to discharge procedures: The prior art discharge measures use different discharge methods to ensure a safe or non-dangerous amount of residual voltage below 0.5V remaining in the energy system / lithium-ion battery, whereby the procedure is designed for lithium-ion battery packs or lithium-ion battery modules. However, the voltage of the lithium-ion battery undergoes voltage recovery after a period of time and reaches a voltage level of up to 40V, whereby the lithium-ion battery pack / module needs to be short-circuited for up to 48 hours after discharge as a waiting / dead time before further processing. Alternatively, the lithium-ion battery can be discharged by using corrosive and aggressive media in a chemical or wet discharge method, thereby reducing and cutting off the electrochemical potential of the lithium-ion battery. However, this method is very slow, uses inorganic and toxic reagents, causes pollution and harmful gas emissions and is mainly applicable to lithium-ion battery cells. In addition, the chemical discharge corrodes the lithium-ion battery from the outside to the inside, resulting in a reduction in the final material yield and quality, the introduction of additional impurities, and the need for post-processing steps for cleaning. Additionally, all currently established prior art discharge methods are greatly limited by the variety and differences of lithium-ion battery packs, modules and cells, and can usually only manage a small portion of this different industry, resulting in long processing and planning times. However, the present invention will achieve an innovative and automated fast discharge route that can handle lithium-ion batteries of different configurations (lithium-ion batteries from different manufacturers, sizes and shapes) at different stages (packs, modules, cells) and overcome long waiting / stagnation times of up to 48 hours by reducing the discharge processing time, while requiring no additional waiting time. The present invention will use a discharge method without relying on a wet chemical discharge method.

[0032] - High yield loss due to shredding: Prior art recycling methods use shredding as a mechanical separation and grinding process to obtain the desired cathode active material or valuable materials such as lithium, cobalt, nickel, manganese inside the lithium-ion battery. Shredding is used and considered a fast and common disassembly method to reduce lithium-ion battery modules or realization materials to particle size and obtain a mixture, whereby material losses of up to 40% are acceptable. The present invention will use efficient, automated and parallelizable (modular) disassembly measures to maintain the maximum possible rate of realization materials input to lithium-ion battery packs, modules and cells (e.g., housings, cables, plugs, battery management systems, etc.). However, the main purpose of the present invention is to obtain high quantity and quality of cathode active materials by abandoning the use of strong mechanical shredding processes and chemical discharge and relying on a piecemeal separation step, which includes disassembling the lithium-ion battery pack to modules, to cells, to cell components, thereby obtaining high purity materials for further recycling processes without the need for powder post-processing steps.

[0033] - Other lithium-ion battery materials / parts are recovered in the form of powder or shredded parts: When using the same lithium-ion battery model, the prior art recycling methods use shredding to obtain black masses of different chemistry and composition due to the use of different input materials or black masses of a single chemistry. In addition, many materials are completely or partially lost in the shredding process, which are not considered cathode active materials, such as electrolytes, separator foils, parts of metal casings, cables, polymers, etc. The currently established recycling processes based on shredding consider these materials and parts to be unnecessary, worthless, or too complex to be recovered for recycling lithium-ion batteries and discard them with a total of at least 20% of the input mass. The present invention will use a disassembly route as described above, whereby all parts will be preserved as much as possible and ideally as they are achieved, whereby these parts do not require any further extensive preparation measures such as methods to filter and sieve them from the shredded mass. These other lithium-ion battery parts will be sorted manually or automatically along the disassembly line into specific material containers, in which all similar parts will be collected and then prepared for further processing / or sale without the need for material powder processing. The method thus has an increased overall recycling share, further reducing energy consumption and carbon gas emissions by eliminating the need to regenerate lithium-ion battery parts.

[0034] - Active materials are usually available only as a powdery agglomerate or black mass, limiting the economic significance and efficiency of recycling: Prior art solutions usually use mechanical treatments such as shredding and inefficient measures to separate or extract cathode active materials from input materials. These methods or processes usually extract only metal powders and black block powder mixtures from the recycling process as the final product. The active material compounds recovered in the black mass have limited economic applications. Limited industrial sectors will benefit from or be interested in the products from these treatments because a large amount of purification or crystallization treatment is required, whereby the original material is considered cheaper and easier to implement into the manufacturing chain. The materials recovered from the current process cannot be fully used for one product or as reusable materials for lithium-ion battery production. The present invention uses a high-purity input cathode active material with particularly low impurities, whereby no additional cleaning steps are required, and the obtained cathode active powder can be chemically treated. An additional post-processing step is provided, which enables the cathode active material to be chemically separated as a large amount and high quality of individual chemical elements, which is mainly attributed to the more appropriate, effective and sustainable pretreatment of lithium-ion batteries (battery packs, modules, cells) by disassembling them part by part, where component integrity is guaranteed.

[0035] -Chemical recovery of cathode materials of lithium-ion batteries based on inorganic treatment: The applied prior art and established methods rely on the use of inorganic substances for different treatments. Inorganic reagents are used from the beginning to the end of the recycling treatment of lithium-ion batteries, because these inorganic reagents are highly reactive and often show high performance. However, the inorganic acids applied are very toxic, leading to dangerous gas development and emissions, causing dangerous wastewater, requiring specially trained staff, equipment and storage facilities. For example, the acidic treatment that has already begun at the time of discharge is also used for hydrometallurgical treatment and post-treatment steps in which recovered materials are obtained. The highly toxic inorganic acids applied are also highly acidic, resulting in complex processing requirements. The present invention does not rely on inorganic acids, but replaces many acidic treatment steps with alternatives, such as for discharge as described above, and realizes alternatives and more environmentally friendly acids such as organic acids. In addition, the inorganic acids used in the chemical separation steps can also be replaced by organic acids, which further reduces the toxic health risks to operators. Therefore, the present application provides a safer and more environmentally friendly recycling treatment for lithium-ion batteries. BRIEF DESCRIPTION OF THE DRAWINGS

[0036] An exemplary embodiment of a lithium-ion battery recycling method according to the present invention is shown in the accompanying drawings, in which:

[0037] Figure 1 : Flow chart of a lithium-ion battery recycling method according to an exemplary embodiment of the present invention.

[0038] Figure 2: Flowchart of step 5 of the method regarding an exemplary embodiment of the present invention.

[0039] The processes in the flow charts are described by vertical lines with capital letters and no numbers along the main process steps and sub-process steps along horizontal lines with capital letters and numbers. The components in the figures are referenced individually as follows.

[0040] A. Preparation of lithium-ion batteries

[0041] A1 State of Health (SoH) Check

[0042] A2 Charging State (SoC) Check

[0043] A3 Lithium-ion battery (pack, module, cell) discharge

[0044] B Disassembly of Lithium-ion Battery Pack

[0045] B1 Remove the cover of the lithium-ion battery pack

[0046] B2 Disassembly and separation of lithium-ion battery pack components

[0047] B2.1 Collect and obtain reusable lithium-ion battery components

[0048] B2.2 Collect and obtain lithium-ion battery modules

[0049] C Disassembly of Li-ion Battery Module

[0050] C1 Open Li-ion battery module

[0051] C2 Disassembly and separation of lithium-ion battery module components

[0052] C2.1 Collect and obtain reusable lithium-ion battery module components

[0053] C2.2 Collect and obtain lithium-ion battery cells

[0054] D Disassembling lithium-ion battery cells

[0055] D1 Open the lithium-ion battery cell

[0056] D2 Removal of electrolyte

[0057] D3 Disassembly and separation of lithium-ion battery cell components

[0058] D3.1 Collect and obtain separators

[0059] D3.2 Collect and obtain anode

[0060] D3.3 Collect and obtain cathode

[0061] E Remove the binder and residual electrolyte from the cathode and anode

[0062] E1 Treatment of cathode and anode by heat treatment

[0063] E2 Separation of active materials and collector foil for anode and cathode

[0064] E2.1 Collect and obtain aluminum foil (cathode collector)

[0065] E2.2 Collect and obtain copper foil (anode collector)

[0066] E2.3 Collect and obtain anode active materials

[0067] E2.4 Collect and obtain cathode active materials

[0068] E3 Clean the anode and cathode collector foils

[0069] F Chemical recovery of anode and cathode active materials

[0070] F1.1 Hydrometallurgical treatment of active materials using organic acids

[0071] F2.1 Recovery of anode active materials

[0072] F2.2 Recovery of cathode active materials

[0073] F2.3 Post-processing to obtain usable anode active materials as precursors

[0074] F2.4 Post-processing to obtain usable cathode active materials as precursors

[0075] G Chemical separation of cathode active materials from lithium-ion batteries

[0076] G1 Separation of cathode active materials for binary lithium-ion battery chemistries

[0077] G1.1 First separation step of cathode active material

[0078] G1.2 Final separation step of cathode active materials

[0079] G2 Separation of cathode active materials for ternary lithium-ion battery chemistries

[0080] G2.1 First separation step of cathode active material

[0081] G2.2 Second separation step of cathode active material

[0082] G2.3 The third separation step of cathode active material

[0083] G2.4 Final separation step of cathode active materials

[0084] GA.1 Extraction and filtration of first separated cathode active materials from lithium-ion batteries

[0085] GA.2 Extraction and filtration of the second separated cathode active material from lithium-ion batteries

[0086] GA.3 Extraction and filtration of third-separated cathode active materials from lithium-ion batteries

[0087] GA.4 Extraction and filtration of final separated cathode active materials from lithium-ion batteries

[0088] GB.1 Post-processing steps for first separation of cathode active materials from lithium-ion batteries

[0089] GB.2 Post-processing step for second separation of cathode active material from lithium-ion batteries

[0090] GB.3 Post-processing steps for the third separation of cathode active materials from lithium-ion batteries

[0091] GB.4 Post-processing steps for final separation of cathode active materials from lithium-ion batteries

[0092] H Drying and Packaging

[0093] J1 Reuse of leachate

[0094] J2 Reuse of the extractant used for the first cathode active material separation process

[0095] J3 Reuse of the extractant used for the second cathode active material separation process

[0096] J4 Reuse of the extractant used for the separation of the third cathode active material

[0097] X1 Discharge Li-ion Battery Pack

[0098] X2 Discharge Li-ion Battery Module

[0099] X3 Discharge Li-ion Battery Cell

[0100] X4 Anode and cathode discharge and removal

[0101] X6 Cathode Active Material

[0102] X7 Recycling cathode active materials

[0103] X8 Individually recovers and separates cathode active material elements

[0104] X9 Leachate with cathode active material ions from lithium-ion batteries

[0105] X10 Leachate with less cathode active material ions

[0106] X11 Leachate with less cathode active material ions

[0107] X12 has a leachate containing only Li ions

[0108] X13 The first recycled material product of lithium-ion batteries

[0109] X14 Lithium-ion battery second recycling material product

[0110] X15 The third recycled material product of lithium-ion batteries

[0111] X16 The product of the final recycled material of lithium-ion batteries

[0112] XP1 Recovering the precursor anode material after leaching

[0113] XP2 Recovering the Precursor Cathode Material after Leaching DETAILED DESCRIPTION

[0114] Overcoming the above industrial challenges and shortcomings of prior art application methods; the following method is proposed and described, especially for lithium-ion battery packs for electric vehicles (EV), while other lithium-ion batteries for other applications, such as electric bicycles, electric scooters, notebooks, mobile phones, etc., or from different configurations, such as modules and cells, can also be recycled by this method. The present invention and process describe a comprehensive method for recycling raw materials from lithium-ion batteries, which include various input streams for EV packs, modules and lithium-ion battery cells. Other types of lithium-ion batteries other than lithium-ion battery EV packs can be integrated into the recycling process stream after pretreatment and discharge in their respective processing steps according to their construction type (such as module (C) or cell (D)). In addition, the present invention can process all common binary lithium-ion battery chemistries such as LCO, LMO, LNO and ternary lithium-ion batteries such as NMC and LNMO with different internal stoichiometric compositions, lithium-ion batteries for different applications and all major lithium-ion battery cell types such as cylindrical, pouch and prismatic cells.

[0115] The present invention relates to a recycling method for lithium-ion batteries, in particular based on dry discharge, in which the discharge energy is reused, disassembly and disassembly into mechanical pretreatment and organic acid leaching for chemical recovery. The method comprises the following steps:

[0116] Step 1: includes a preparation step (A) of a diagnostic tool and a discharge step (preferably dry discharge) of a lithium ion battery (A3).

[0117] Step 2: Disassembly, disassembly, separation and collection process for lithium-ion batteries, which includes disassembling the lithium-ion battery casing, disassembling the lithium-ion battery piece by piece without any crushing or shredding of any materials involved, and thereby separating and collecting all related parts into lithium-ion battery cell components, such as cathodes (positive electrodes) with their corresponding active material compositions, anodes (negative electrodes) with their corresponding active material compositions, separators and electrolytes; followed by collecting other undamaged and reusable materials implemented in the lithium-ion battery system, such as battery packs, casings, cables, PMS, PCBs (B, C and D).

[0118] Step 3: Removing the binder (E) between the anode and cathode by thermal, mechanical or chemical treatment or by any combination of these methods to separate the active materials of the cathode and / or anode individually from their respective metal collector foils without introducing any impurities or severe degradation and removing any residual electrolyte.

[0119] Step 4: Chemically recover the active materials (F) of the cathode and anode, respectively, with high yields using environmentally friendly hydrometallurgical operations, such as leaching in an organic acid solution (F1) with or without a reducing agent to obtain a leachate in which all target materials (e.g., cathode active material metals) of the input material are completely or partially dissolved; wherein the chemical recovery of the active materials is sustainable to obtain active material components alone or to obtain chemical precursor reagents for anode or cathode materials.

[0120] Step 5: The cathode and anode active materials within the leachate are chemically separated and processed into their individual chemical elements as separate products, respectively, by a stepwise process using reusable reagents (G).

[0121] Step 6: Cleaning, drying, packaging (H) and preparation of materials obtained and separated from recycling process as finishing step of lithium ion battery recycling process. The product obtained after the final step is ready for reuse, resale or further processing as a product.

[0122] In step 1, preparation of the lithium-ion battery for discharge treatment (A) is performed in order to reduce the risk of thermal runaway, fire or other possible dangerous potentials during the treatment process; thus, the lithium-ion battery is relieved of its charging and threat potential. This step (step 1) takes into account lithium-ion battery packs, modules and cells, and includes at least the following preferred discharge procedures:

[0123] Health status check (A1); it includes at least one of optical and / or electrical and / or mechanical checks to classify the lithium-ion battery and determine its state for further processing. This processing step is important to determine whether the lithium-ion battery is healthy, to determine its construction type, its implementation technology, and therefore to determine the most suitable and efficient processing route, or more precisely to determine the required discharge settings. In a preferred embodiment, based on the results of the health status check, it is determined whether the lithium-ion battery is suitable for recycling or whether it can be used for a second life use.

[0124] State of charge check (A2); where the state of charge of the lithium-ion battery is analyzed to determine the remaining electrical energy / residual voltage still stored / available in the lithium-ion battery. This analysis gives the necessary information on the parameters of the subsequent discharge step; like the required duration and the discharge current to be applied.

[0125] The lithium-ion battery (A3) is discharged by an electrical device, wherein preferably a current of 2 to 20 amperes and a duration of 1 to 120 minutes are applied to discharge the lithium-ion battery. The amount of current and the duration of discharge within given limits are determined with reference to the previous step; the amount of residual electrical energy is stored in the lithium-ion battery according to the determined amount. The lithium-ion battery is preferably discharged at a critical voltage level for 2 volt processing, and most preferably each lithium-ion battery module is discharged to a voltage level of about 0.5V. If the lithium-ion battery is not discharged to below the critical integrity voltage level (which is about 0.5V), the handling of the lithium-ion battery will be too dangerous due to the risk of thermal runaway, short circuit and combustion during further processing. In a preferred embodiment, the discharge energy available in step 1 will be directly used to power other steps of the recycling process, be reintroduced into the power grid, used to charge other applications of the lithium-ion battery (e.g., second life applications), or used for other applications (like EV charging stations), whereby the discharge energy will not be lost.

[0126] The entire step 1 (A) or at least the step of discharging the lithium-ion battery (A3) is partially or fully automated. In addition, special pre-treatment is required for lithium-ion batteries introduced into recycling processing as lithium-ion battery packs. The lithium-ion battery pack needs to be opened, and the lithium-ion battery modules need to be disconnected from the lithium-ion battery pack in order to discharge each single lithium-ion battery module of the lithium-ion battery pack, thereby ensuring safe handling and bypassing the BMS of the battery pack while keeping the structural integrity of the lithium-ion batteries intact. Opening the lithium-ion battery pack can be performed manually or automatically by releasing joints, closures, screws and / or cutting the closed casing. During the health status check (A1), the appropriate method will be determined from the preparation step (step 1).

[0127] After step 1, the discharged lithium-ion batteries (group: X1, module: X2, cell: X3) are manually or automatically transferred to the corresponding disassembly processing steps given in step 2 above (group: B, module: C, cell: D).

[0128] The entire step 2 of the EV lithium-ion battery pack preferably includes the following sub-steps:

[0129] disassembling and disassembling the lithium-ion battery into lithium-ion battery modules (B), which are collected and obtained next to other reusable lithium-ion battery components;

[0130] disassembling and disassembling the lithium-ion battery modules into lithium-ion battery cells (C) collected and obtained alongside other reusable lithium-ion battery module components;

[0131] Disassembling and disassembling lithium-ion battery cells down to lithium-ion battery cell components (D), such as cathode, anode, separator and electrolyte, with minimal impact on battery component integrity, high yield and purity.

[0132] As will be given in detail, during the disassembly process the lithium-ion batteries are mainly decomposed by mechanical means, but the process can be supported by thermal and / or optical systems and similar thermal, thermomechanical, chemical, thermochemical or mechanochemical means.

[0133] Disassembly and dismantling of lithium-ion battery packs (B) into lithium-ion battery modules: In order to save recyclable and valuable lithium-ion battery pack components such as aluminum, steel, copper, cables, electronic devices, plastics, etc., manual or automatic disassembly and dismantling of lithium-ion battery packs is required. The procedure includes:

[0134] - When the lithium ion battery housing is opened, the cover is manually or automatically removed and collected, thereby exposing the interior and components of the lithium ion battery (B1).

[0135] - disassembling and separating the lithium-ion battery components (B2); which includes manually or automatically sorting the components into

[0136] o Further recyclable or reusable lithium-ion battery components (B2.1): for example, copper, aluminum, cables, plastics, mixed metals, and other parts other than modules that are further sorted, processed, and prepared for reuse in other applications (e.g., as refinishing) or for sale.

[0137] o Lithium-ion battery modules (B2.2): After the identification of non-critical voltages based on possible voltage relaxation effects, the internal voltage of the discharged lithium-ion battery modules (X2) is checked again and conveyed (manually or automatically) to the next recycling process step (C). Lithium-ion battery modules are components that require further disassembly and processing in order to reach the lithium-ion battery cells in which valuable materials are realized.

[0138] Disassembly and removal of Li-ion battery modules (C) into Li-ion battery cells: Manual or automated disassembly of Li-ion battery modules is required to further preserve recyclable and valuable components. In addition, Li-ion battery cells and cell component materials must be reached without damaging, degrading or contaminating them, as these are the most valuable materials of Li-ion batteries. The process includes:

[0139] - Manual or automatic opening of the lithium-ion battery module (C1);

[0140] - Manual or automatic disassembly and separation of lithium-ion battery module components (C2) into

[0141] o Other recyclable or reusable components (C2.1): e.g. copper, aluminium, cables, plastics, mixed metals, etc., which are further sorted and processed;

[0142] o Lithium-ion battery cells (C2.2) that can have one of three different shapes / configurations: pouch, prismatic, cylindrical. The discharged lithium-ion battery cells (X3) are transported manually or automatically to the next recycling process step (D). Lithium-ion battery cells are components that require further disassembly and processing to obtain anodes, cathodes and other components with valuable materials therein.

[0143] Disassembling and disassembling lithium-ion battery cells (D) into lithium-ion battery cell components such as cathodes, anodes, separators and electrolytes: In order to save large quantities and high quality of valuable components and materials and to minimize the required processing steps, manual or automated disassembling and disassembling of lithium-ion battery cells is required. By utilizing processing steps such as disassembling and disassembling and not relying on shredding, processing steps such as magnetic separation, screening and flotation can be discarded. In addition, if the quality and purity of input materials such as anodes and cathodes are obtained at the highest possible purity level, subsequent chemical processing will achieve higher yields and purity, which is possible with disassembly and disassembly. The process includes:

[0144] - Manual or automatic opening of lithium-ion battery cells (D1) in a protected and closed environment to prevent the release of harmful gas emissions and as a safety precaution against other threats.

[0145] - Extraction or removal of the electrolyte (D2) by washing the opened cell with a liquid, using a supercritical fluid, or using CO2 gas, or by thermal measurement, when the lithium-ion battery cell is opened and the separator foil has been removed before the thermal measurement, for example by heating for a period of time at elevated temperature in a vacuum oven or furnace under an inert gas atmosphere. For further processing of the active materials of the anode and cathode based on the liquid state of the electrolyte, extraction and removal of the electrolyte is required, which will interfere with the subsequent separation process. The electrolyte does not necessarily need to be obtained or recovered, but needs to be removed before further processing.

[0146] - Disassembly and separation of lithium-ion battery cell components (D3): When the electrolyte is extracted, the internal components of the lithium-ion battery cell are separated from the outer casing using non-thermal pretreatment in (D2); the parts / products are separated and classified into:

[0147] oSeparator (D3.1): The separator is a plastic component in the lithium-ion battery cell that prevents short circuits during the charge and discharge process. After separation, the separator can be collected and further processed.

[0148] o Anode (D3.2): The anode is the negative collector of the lithium-ion battery cell, receiving lithium ions from the cathode during the charging process. The main components of the anode are the collector foil (usually copper), the binder (usually PVFD) and the active material (usually a graphite component, or a silicon component). The anode is taken to the next processing step to remove the binder connecting the collector foil and the active material; and

[0149] o Cathode (D3.3): The cathode is the positive collector of the lithium-ion battery cell and transfers lithium ions to the anode during the charging process. The main components of the cathode are the collector foil (usually aluminum), the binder (usually PVFD) and the active material (different compositions of Ni, Mn, Co, Fe, P, Li, or basically LCO, LNO, LMO, NMC in our case). The cathode is taken to the next processing step to remove the binder connecting the collector foil and the active material.

[0150] - Preferably (manually or automatically) conveying the discharged and disassembled anodes and cathodes (X4) to the next main treatment step (E).

[0151] The stepwise manual or automatic disassembly and disassembly of lithium-ion batteries as described above is necessary to preserve valuable components and active materials (cathode and anode, etc.), which are targeted for recycling and need to be recovered so that they can be reused and further improve recycling efficiency and effectiveness. In addition, disassembly and disassembly are required to obtain the highest material input and quality of battery cell components such as anodes, cathodes and other components. In order to improve the purity of the elements finally recovered, it is necessary to separate the lithium-ion battery battery cell components (separators, electrolytes, anodes, cathodes) to obtain a separate processing flow for anode and cathode active materials.

[0152] In step 3, the binder (E) between the anode and cathode is removed to separate the active materials of the cathode and / or anode from their respective metal collector foils for further recovery of the active materials in a chemical organic leaching process. In addition to removing the binder, some residual electrolyte within the respective anode and cathode will also be removed. This step preferably comprises the following sub-steps:

[0153] - Heat treatment (E1): Thermal dissolution at high temperature is important in order to 1) remove the binder and 2) increase the surface of the valuable active material elements and 3) remove any residual electrolyte. The binder can be dissolved / evaporated with a thermal procedure such as pyrolysis by heating the anode and cathode compositions to a temperature between 250° C. and 650° C. in a vacuum or inert gas atmosphere furnace and maintaining these temperatures at a temperature increase rate (heating rate) of 5 to 15° C. per minute for a duration of 10 to 120 minutes, wherein a nitrogen flow is used if necessary.

[0154] - Separation of active materials and collector foils (E2): After the removal of the binder, the anode and cathode are treated to separate their active materials from the respective metal collector / foil. This separation can be performed mechanically, chemically, by gravity or any combination thereof. That is, for example: the separation can be by scraping off the active material or shaking it off the collector (mechanical treatment) or by washing the active material in a water bath or stream (chemical treatment) and continuous drying. After the separation of the active materials of the anode and cathode from their respective collector foils, the components are sorted into parts / products as follows:

[0155] o Aluminum foil from cathode collector (E2.1),

[0156] o Copper foil from anode collector (E2.2),

[0157] o Anode active materials consisting of graphite or silicon compositions (E2.3),

[0158] o cathode active material (E2.4), for example composed of a combination of chemical elements such as nickel, manganese, cobalt and lithium, but not limited to these chemical elements;

[0159] - Cleaning treatment of the obtained collector foils of the anode and cathode (E3): Before packaging and sale, the separated collector foils need to be cleaned to increase the material value. This can be done by washing them in distilled / deionized water with or without ultrasound assistance. Aluminum and copper foils are treated in this step.

[0160] Preferably, the obtained anode active material (X5) and cathode active material (X6) are manually or automatically conveyed to the next processing step (F) and processed separately.

[0161] Manual or automatic separation of lithium-ion battery cell active materials from their collector foils is necessary in order to save valuable components and active materials in large quantities and high quality without further processing steps; the separated active materials can thereby be introduced directly into their respective processing streams.

[0162] In step 4, chemical recovery of the active materials of the cathode and anode (F) is provided. The chemical organic recovery of the active materials is achieved by dissolving the solid matter of the active materials obtained in a reusable leachate (J1), from which the individual materials can be recovered, thus increasing the value of the materials recovered from the recycling process as reusable materials. The chemical recovery of the anode (graphite, silicon or other) and the cathode material (for example, a composition based on nickel, cobalt, manganese, lithium) is carried out in separate reactors, in physically separate processes that are independent of each other and not combined, where cathode materials with similar chemical properties such as NMC and LCO are miscible. The chemical recovery preferably consists of the following operations:

[0163] -Hydrometallurgical treatment with organic acids (F1.1) such as citric acid, malic acid and / or formic acid as leaching agents: Leaching the active material with organic acids improves the environmental impact and treatment efficiency. It produces less harmful gases, while it improves the recycling efficiency and has lower toxicity. The concentration of the leaching agent in the leaching solution is preferably set to 0.5M-3.0M. The leaching treatment is carried out at a temperature of 60.1°C to 99.9°C for a duration of 15 to 120 minutes. The solid / liquid ratio is set to 10-120 g / L. This organic leaching treatment may or may not be accompanied by an organic or inorganic reducing agent to improve the recycling efficiency, output rate and treatment performance. The reducing agent includes at least one of hydrogen peroxide, sodium thiosulfate, sodium bisulfite, D-glucose, sucrose or ascorbic acid, and is added to the leaching solution at a concentration of 0.1-10% by volume. The following materials are obtained from this treatment:

[0164] o The anode active material (F2.1) recovered from the anode leaching process, which is graphite or silicon or a mixed graphite and silicon composition, and can be processed into a precursor (F2.3), which can be manually or automatically transferred to a drying and packaging step (H), where the final anode active material product, such as graphite or silicon or a mixed graphite and silicon product (XP1) is obtained.

[0165] o Cathode active material (F2.2) recovered from the cathode leaching treatment; it consists of a combination of different cathode active material components that can be processed into a precursor that can be considered as a final reusable product (F2.4), extracted from the process chain and manually or automatically transferred to a drying and packaging step (H), where a precursor material with a fixed stoichiometric composition (XP2) is obtained and can be further used in the production of new lithium-ion battery cells with limited use of the same composition ratio / stoichiometric composition. However, in order to improve availability, it is preferred to further process the recovered cathode active material (F2.2) in a separation treatment (G). In this case, it is preferred to transfer the recovered cathode active material (X7) to the next treatment (G).

[0166] The chemical recycling process can be applied to Li-ion batteries from one source or application, while it can also be applied to mixed Li-ion battery streams from different applications and chemistries, such as NMC-111, NMC-811, NMC-532, etc., or chemistries that depend on the elements present in the NMC chemistry, such as LCO, LNO, LMO batteries.

[0167] After step 4, the recovered / leached cathode active material (X7) can be manually or automatically transported to the next processing step; step 5; the recovered cathode active material composition is separated into its chemical elements to increase the reusability and flexibility of processing the output material. Therefore, after step 4, the following step 5 is performed on the recovered cathode active material:

[0168] Step 5: Chemical separation of cathode active materials from lithium-ion batteries (G) is performed in any order by sequential chemical separation procedures of target materials from metal ions such as lithium, nickel, cobalt and / or manganese from the leaching mother solution ( Figure 2 The exemplary embodiments given in are not bound to the separation sequence, but distinguish between the recycling of separate binary and ternary systems which include additional extraction work-up steps), which include the following:

[0169] - Sequential separation of each metal from the leachate to obtain a carrier solution with the target metal ions (binary system only: G1.1 and G1.4, otherwise G2.1 to G2.4);

[0170] - transfer of the target metal from the first support / extraction solution into the second support solution (binary systems only: GA.1 and GA.4, otherwise GA.1 to GA.4) and obtaining the previously applied reagents (J2, J3, J4) required for the production of the first support / extraction solution, whereby the reagents can be recovered and reintegrated into the chemical extraction process (in G);

[0171] - Obtaining the target metal from the second carrier solution and performing a filtration treatment to separate the obtained solidified / precipitated metal material from the second carrier solution (only for binary systems: GB.1 and GB.4, otherwise GB.1 to GB.4).

[0172] In a preferred embodiment, the chemical separation of the cathode active material elements comprises the following:

[0173] - Sequentially separating the metals individually from the leachate to obtain a first support solution having only one target metal ion type;

[0174] - separating the first carrier solution from the residual leachate;

[0175] - Transferring the target metal from the extracted first carrier solution to the second carrier solution and obtaining the previously applied extractant for reuse;

[0176] - The target metal is obtained as a solid residue from the second support solution by precipitation and filtration.

[0177] In another preferred embodiment, the chemical separation of the cathode active material elements comprises:

[0178] - Sequentially separate the metals from the leachate individually to obtain a solid residue having only one target metal ion type in the solid residue compound;

[0179] - filtering the solid residue from the residual leachate;

[0180] - Transferring the target metal from the solidified residue into the carrier solution and obtaining the previously applied extractant for reuse;

[0181] - The target metal is obtained as a solid residue from the support solution by precipitation and filtration.

[0182] In a preferred embodiment of the present invention, Figure 2 As shown; Step 5, which is the chemical separation of the cathode active material element (G), comprises the following steps:

[0183] - Separation of cathode active materials for binary lithium-ion battery chemistries (G1): This separation process is used for cathode active material compositions based on lithium and another transition metal (eg cobalt or manganese or nickel).

[0184] o First separation step (G1.1) of cathode active material; separation of transition metals from the leachate.

[0185] o Final separation step of cathode active material (G1.2); extraction of lithium from the residual leachate.

[0186] - Separation of cathode active materials for ternary lithium-ion battery chemistries (G2): This separation process is used for cathode active material compositions based on a combination of lithium and transition metals such as cobalt, nickel and / or manganese.

[0187] o First separation step (G2.1) of cathode active material: separation of a transition metal from the leachate.

[0188] o Second separation step (G2.2) of cathode active material; separation of another transition metal from the leachate.

[0189] o Third separation step (G2.3) of cathode active material: separation of another transition metal from the leachate.

[0190] o Final separation step of cathode active material (G2.4); extraction of lithium from the residual leachate.

[0191] like Figure 2 As shown, an exemplary leachate (X9) containing a ternary lithium-ion battery chemistry having nickel, cobalt, manganese and lithium ions comes from a chemical recovery (F2.2) step of the cathode active material; and with the separation of the first transition metal, the remaining leachate (X10) carries one less type of transition metal; the leachate after the second separation (X11) carries two less transition metals, and the leachate before the final separation (X12) carries only or primarily lithium ions.

[0192] In step 5, the chemical separation process (G) of the valuable metals (cathode active material elements) from the leachate is divided into a separation step for each chemical element present in the mother leachate. The separation can be performed by direct precipitation from the leachate into a solidified compound and / or by solvent extraction (liquid-liquid extraction) in any order. In a preferred embodiment, after filtering and separating one component from the leachate, the previous solution is divided into a carrier solution or precipitate and a residual leachate, which will be further used in the next process step to separate the remaining chemical elements from the leachate.

[0193] The following extractants can be used together with the phase stabilizer tributyl phosphate (TBP) and the diluent kerosene (with varying concentrations or volume content) for separating valuable metals from the leachate:

[0194] Chemical extractants, diluents and solvents for liquid-liquid extraction:

[0195] -Cyanex272,

[0196] -D2EHPA,

[0197] -PC88A,

[0198] -Versatic10 Neodecanoic Acid,

[0199] -Trioctylphosphine oxide (TOPO),

[0200] -Benzoyltrifluoroacetone (HBTA)

[0201] -Trioctylamine (TOA),

[0202] Chemical precipitation extractants do not require phase stabilizers and kerosene as a diluent.

[0203] Chemical extractants used for precipitation:

[0204] - dimethylglyoxime (DMG),

[0205] -Sodium phosphate, sodium sulfate, sodium hydroxide, sodium carbonate,

[0206] -Ammonium oxalate.

[0207] In a preferred embodiment, step 5 includes at least one of the "Separation of cathode active materials for binary lithium-ion battery chemistry" (G1) or "Separation of cathode active materials for ternary lithium-ion battery chemistry" (G2) active material treatments given below with the following sub-steps and details:

[0208] Separation (G1) of cathode active materials of binary lithium-ion battery chemistries, exemplified by LCO (LiCoO2), in which the transition metal cobalt is primarily extracted from the leachate, followed by the extraction of lithium. However, the reverse treatment of first extracting lithium, then extracting cobalt, and then finally extracting lithium is also possible, however different optimized treatment conditions are selected. The separation step includes recovering the metal ions from the leachate into an organic phase by chemical reaction or direct precipitation, whereby the resulting solution or compound with the extracted metal ions is separated from the remaining leachate solution carrying the remaining transition metals and further treated to separate other metal ions. The separated solution or compound with the recovered metal ions is further treated in an extraction and filtration step to transfer the target metal to another phase and to recover the reagents originally used for the solvent extraction treatment. The recovered metal ions are then precipitated, filtered and obtained as a compound that can be further treated in a post-treatment step. The above method can also be used for other binary lithium-ion battery chemistries, such as LNO and LMO, where the separation treatment of each transition metal can be obtained from the treatment of ternary lithium-ion batteries described below. In detail, the recovery of LCO from the cathode active material in the leachate includes:

[0209] - Cobalt is selectively separated from the leach solution (G1.1) by precipitation or solvent extraction. Depending on the chosen method, other reagents / extractants can be used. For example, ammonium oxalate (0.1-2 mol / L) selectively precipitates hydrated cobalt oxalate (CoC2O4·2H2O). The optimal treatment conditions under constant stirring and heating in the reactor are given by the following formula: the temperature is between 15-30°C and the pH level is between 4-7. The chemical reaction time is 20-90 minutes long. Alternatively, cobalt is separated from the leach solution by solvent extraction (GA.1). For this purpose, chemical extractants such as Cyanex 272, PC-88A and / or Cyanex 272 with tributyl phosphate (TBP) can be used to selectively extract cobalt. The chemical reaction occurs between 3-6.5 pH. The resulting cobalt oxalate hydrate or the organic solution containing the extracted metal in ionized form is then separated from the residual leachate (GA.1) containing other metal ions by filtration or other means. Afterwards, the separated medium carrying the first extracted cathode active material (solid or liquid) is treated with an acid such as sulfuric acid and then with sodium carbonate or sodium sulfate as part of a post-treatment (GB.1).

[0210] -Lithium is selectively separated from the leachate solution (G1.2) preferably by precipitation, but can also be treated by solvent extraction. As a chemical reagent, saturated sodium carbonate can be used at a temperature of about 100°C, at pH = 11-13 for a duration of 20-60 minutes, ideally with a molar ratio of lithium ions to sodium carbonate between 0.2 and 1.5, to directly treat the leachate carrying lithium ions (GB.4). Another chemical reagent for separating lithium from the leachate is 0.2 to 2 mol / L sodium phosphate. Lithium can be extracted by DEHPA with 0.06 mol·L-1DEHPA, organic to -aqueous solution ratio (O / A) = 1:1 and pH = 2-4. Alternatively, lithium is extracted from the leachate under the conditions of pH = 7-9, 0.4 mol·L-1HBTA + 0.4 mol·L-1TOPO + kerosene, O / A = 1:1, 70% saponification and extraction for 2 minutes. The lithium-carrying solution (GA.4) is then filtered and separated from the residual leachate and treated with sodium carbonate in a post-treatment (GB.4).

[0211] Separation of cathode active materials for ternary lithium-ion battery chemistries (G2), where the separation order of transition metals nickel, cobalt and manganese is variable. Therefore, the following possible separation order is possible:

[0212]

[0213] However, lithium is often extracted last, but there are also extraction conditions whereby lithium can be extracted first and then extracted again as the last extraction step. The following description describes a separation process for a ternary lithium-ion battery having a cobalt-nickel-manganese-lithium separation sequence, wherein the arrangement method for each individual material can also be used for other sequences. The separation step includes recovering the metal ions from the leachate into an organic phase by chemical reaction or direct precipitation, thereby separating the resulting solution or compound with the extracted metal ions from the remaining leachate solution carrying the remaining transition metals, and further processing to subsequently separate other metal ions. The separated solution or compound with the recovered metal ions is further processed in an extraction and filtration step to transfer the target metal to another phase and recover the reagents originally used for the solvent extraction process. The recovered metal ions are then precipitated, filtered and obtained as compounds that can be further processed in a post-processing step. The above-mentioned treatment can be used for a mixture of binary and ternary lithium-ion battery chemicals or only for ternary lithium-ion batteries. In detail, the recovery of cathode active materials from the leachate of at least a ternary lithium-ion battery includes:

[0214] A separation step or direct precipitation of the transition metal to an organic phase (G2.1, G2.2, G2.3, G2.4), with an extraction and filtration step of a solution or compound of the separated metal ions (GA.1, GA.2, GA.3, GA.4) to transfer the target metal to another phase and recover the reagents originally used for the solvent extraction process. The extracted metal ions are then obtained as compounds by a post-treatment step (GB.1, GB.2, GB.3, GB.4). For an exemplary separation sequence of ternary lithium-ion battery chemistries of NMC and cobalt-nickel-manganese-lithium, the following procedures are exemplarily described:

[0215] - Cobalt is selectively separated from the leach solution (G2.1) by precipitation or solvent extraction. Depending on the method chosen, other reagents / extractants can be used. For example, ammonium oxalate (0.1-2 mol / L) selectively precipitates hydrated cobalt oxalate (CoC2O4·2H2O). The optimal treatment conditions under constant stirring and heating in the reactor are given by the following formula: the temperature is between 15-30°C and the pH level is between 4-7. The chemical reaction time is 20-90 minutes long. Alternatively, cobalt is separated from the leach solution by solvent extraction (GA.1). For this purpose, chemical extractants such as Cyanex272, PC-88A and / or Cyanex272 with tributyl phosphate (TBP) can be used to selectively extract cobalt. The chemical reaction occurs between 3-6.5 pH. The resulting cobalt oxalate hydrate or the organic solution containing the extracted metal in ionized form is then separated from the residual leachate (GA.1) containing other metal ions by filtration or other means. Afterwards, the separated medium carrying the first extracted cathode active material (solid or liquid) is treated with an acid such as sulfuric acid and then with sodium carbonate or sodium sulfate as part of a post-treatment (GB.1).

[0216] -Selective separation of nickel from the leaching solution / leaching liquor by adding a reagent / extractant (G2.2). Nickel is extracted by dimethylglyoxime (DMG) at a concentration of 0.02-0.2 mol / L in a temperature range of 15-30°C and a pH range of 4-5 or 7.4 to 10 for 5 minutes to 60 minutes. After the chemical reaction, the nickel ion solution is extracted and filtered (GA.2), whereby a nickel product is obtained by post-treatment (GB.2). Post-treatment (GB.2) includes treatment with 3 mol / L-5 mol / L hydrochloric acid or sulfuric acid. Then, nickel is selectively separated with 1-3 mol / L ammonium hydroxide at a pH range of 2.5-5 or by sodium carbonate or sodium sulfate.

[0217] - Selective separation of manganese from the leach solution via precipitation or solvent extraction (G2.3). Manganese ions are separated from the leach solution (GA.3) by using chemical reagents such as di-(2-ethylhexyl)phosphoric acid (D2EHPA) and sulphonated kerosene. D2EHPA is saponified 60-85% with concentrated sodium hydroxide (5-13 mol / L). In addition, 1-8% by volume of tributyl phosphate is used. The organic phase loaded with manganese (GA.3) is separated and filtered from the leach solution, thereby recovering the applied extractant. The resulting manganese-loaded solution is treated with an inorganic acid solution such as sulphuric acid and then with sodium carbonate or sodium sulphate as part of a post-treatment step (GB.3).

[0218] -Lithium is selectively separated from the leachate solution (G2.4) preferably by precipitation, but can also be treated by solvent extraction. As a chemical reagent, saturated sodium carbonate can be used at a temperature of about 100°C, at pH = 11-13 for a duration of 20-60 minutes, ideally with a molar ratio of lithium ions to sodium carbonate between 0.2 and 1.5 to directly treat the leachate carrying lithium ions (GB.4). Another chemical reagent for separating lithium from the leachate is 0.2 to 2 mol / L sodium phosphate. Lithium can be extracted by DEHPA with 0.06 mol·L-1DEHPA, organic to -aqueous solution ratio (O / A) = 1:1 and pH = 2-4. Alternatively, lithium is extracted from the leachate under the conditions of pH = 7-9, 0.4 mol·L-1HBTA + 0.4 mol·L-1TOPO + kerosene, O / A = 1:1, 70% saponification and extraction for 2 minutes. The lithium-carrying solution (GA.4) is then filtered and separated from the residual leachate and treated with sodium carbonate in a post-treatment (GB.4).

[0219] The cathode active materials (X13, X14, X15, X16) separated and extracted from each separation step obtained after post-treatment (GB.1, GB.2, GB.3, GB.4) are transferred to the next processing step, i.e. step 6, drying and packaging step (H), manually or by automated means.

[0220] After step 5, in a drying and packaging step (H), final treatment is performed; wherein a drying treatment of the separated active material elements (X13, X14, X15, X16) and / or the obtained precursor materials (XP1, XP2) is performed. The drying treatment is preferably performed in a sealed device to inhibit oxidation and agglomeration, for example in a vacuum furnace or an inert gas furnace, whereby the final product / element is automatically or manually packaged into an airtight bag. In a preferred embodiment, the drying duration is set to a time period of 0.5 to 8.0 hours, and the drying temperature is set between 50°C and 250°C and preferably to 70°C. Preferably, the drying environment is under an inert gas such as argon or nitrogen at standard atmospheric pressure.

Claims

1. A method for recycling lithium-ion batteries, characterized in that The following processing: - a preparation step which comprises a diagnosis of the lithium-ion battery, followed by opening the lithium-ion battery pack and discharging the lithium-ion modules and / or cells, - for the disassembly and disassembly process of lithium-ion batteries, which includes disassembling the lithium-ion battery casing and disassembling the lithium-ion battery down to its cell components to obtain the cathode with its corresponding active material composition, the anode with its corresponding active material composition, the separator and the electrolyte; as well as the collection of other parts implemented in the lithium-ion battery energy system, - removing the binder between the anode and cathode foils and their respective active material compositions to separate the anode and cathode collector foils from their respective active materials individually; - Chemical recovery of the separated active materials of the cathode and anode, respectively, by hydrometallurgical operations; - Individual and subsequent chemical separation and processing of the cathode active materials down to their individual chemical elements as separate products.

2. The method of recycling lithium-ion batteries according to claim 1, wherein the initial preparation step comprises: - State of health checks to determine if a lithium-ion battery is suitable for recycling, to identify the build type and geometry, and to prepare the required digital data set for subsequent discharge processing; - a state of charge check in order to determine the remaining electrical energy / residual voltage still stored in the lithium-ion battery and thus the necessary processing parameters for the subsequent discharge step; - Discharging the lithium-ion battery module by means of an electrical device with a discharge current and a discharge duration corresponding to the data obtained in the health status / charge check.

3. The method for recycling lithium-ion batteries according to claim 1 or 2, wherein the disassembly and disassembly process of the lithium-ion batteries comprises the following sub-steps: - Dismantle and disassemble lithium-ion battery packs into lithium-ion battery modules, collect reusable parts and obtain lithium-ion battery modules; - Disassemble and disassemble lithium-ion battery modules into lithium-ion battery cells, collect reusable parts and obtain lithium-ion battery cells; - Disassembling and disassembling lithium-ion battery cells down to lithium-ion battery cell components to obtain lithium-ion battery cell components such as cathodes, anodes, separators and electrolytes.

4. The method of recycling lithium-ion batteries according to claim 3, wherein the lithium-ion batteries are disassembled and disassembled using at least one of mechanical, thermal, thermomechanical, chemical, thermochemical or mechano-chemical means or any other combination of these methods.

5. A method of recycling lithium ion batteries according to any one of the preceding claims, wherein the removal of the binder and residual electrolyte comprises: - heat treatment to remove the binder and any residual electrolyte; - Separation of anode and cathode active materials from collector foil; - The components are sorted into collector foil, cathode active material and anode active material.

6. A method of recycling lithium-ion batteries according to any one of the preceding claims, wherein the chemical recovery of the anode and cathode active materials is carried out in physically separate processes that are independent of each other and cannot be recombined.

7. A method for recycling lithium-ion batteries according to any one of the preceding claims, wherein the hydrometallurgical operation comprises leaching the active materials individually in an organic acid solution to obtain a leachate having all target metals of the corresponding anode or cathode active material input composition.

8. The method for recycling lithium-ion batteries according to claim 7, wherein the leaching is performed with an organic acid solution comprising at least one of citric acid, formic acid and / or malic acid.

9. A method of recycling lithium-ion batteries according to claim 7 or 8, wherein the hydrometallurgical or organic leaching treatment is accompanied by an organic or inorganic reducing agent.

10. The method of recycling lithium ion batteries according to claim 9, wherein the reducing agent comprises at least one of hydrogen peroxide, sodium thiosulfate, sodium bisulfite, D-glucose, sucrose or ascorbic acid.

11. A method of recycling lithium ion batteries according to any one of claims 7 to 10, wherein the chemical separation of cathode active material or anode material comprises a separate chemical separation of cathode or anode active material from a leachate.

12. The method of recycling lithium ion batteries according to claim 11, wherein the chemical separation of cathode active material elements is performed by continuous chemical separation / extraction of target metals from a leaching mother solution having at least one of metal ions of lithium, nickel, cobalt and / or manganese, by solvent extraction or direct precipitation in any order.

13. A method of recycling lithium ion batteries according to claim 11 or 12, wherein the chemical separation of the cathode active material elements comprises: - Sequential separation of metals from the leachate individually to obtain a carrier solution with only one target metal ion type or using a direct precipitation method to obtain a residue carrying metal ions; - separating the carrier solution or residue from the leachate; - Transferring the target metal from the extracted carrier solution or residue into another solution and obtaining the previously applied extractant for reuse; - The target metal is obtained as a solid residue from the solution by precipitation and filtration.

14. A method for recycling lithium-ion batteries according to any one of claims 11 to 13, wherein after filtering and separating one material from the leachate, the former solution is separated into a precipitate and a residual leachate, which are further used in the next processing step to separate the remaining components.

15. The method for recycling lithium-ion batteries according to any of the preceding claims, wherein the lithium-ion battery is any lithium-ion battery assembly, such as a pack or module for different applications, and / or any lithium-ion battery cell of any of the following cell types, cylindrical, pouch or prismatic.

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