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WO2025012520A1 - Procédé et appareil de recyclage de batterie - Google Patents

Procédé et appareil de recyclage de batterie Download PDF

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Publication number
WO2025012520A1
WO2025012520A1 PCT/FI2024/050389 FI2024050389W WO2025012520A1 WO 2025012520 A1 WO2025012520 A1 WO 2025012520A1 FI 2024050389 W FI2024050389 W FI 2024050389W WO 2025012520 A1 WO2025012520 A1 WO 2025012520A1
Authority
WO
WIPO (PCT)
Prior art keywords
battery
active materials
mixture
anode
active material
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Pending
Application number
PCT/FI2024/050389
Other languages
English (en)
Inventor
Annukka SANTASALO-AARNIO
Neha Garg
Aravindda Swamy VENKATESH
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Aalto Korkeakoulusaatio sr
Original Assignee
Aalto Korkeakoulusaatio sr
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Aalto Korkeakoulusaatio sr filed Critical Aalto Korkeakoulusaatio sr
Publication of WO2025012520A1 publication Critical patent/WO2025012520A1/fr
Pending legal-status Critical Current
Anticipated expiration legal-status Critical

Links

Classifications

    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
    • C22B26/00—Obtaining alkali, alkaline earth metals or magnesium
    • C22B26/10—Obtaining alkali metals
    • C22B26/12—Obtaining lithium
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B09—DISPOSAL OF SOLID WASTE; RECLAMATION OF CONTAMINATED SOIL
    • B09B—DISPOSAL OF SOLID WASTE NOT OTHERWISE PROVIDED FOR
    • B09B3/00—Destroying solid waste or transforming solid waste into something useful or harmless
    • B09B3/30—Destroying solid waste or transforming solid waste into something useful or harmless involving mechanical treatment
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
    • C22B1/00—Preliminary treatment of ores or scrap
    • C22B1/005—Preliminary treatment of scrap
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
    • C22B23/00—Obtaining nickel or cobalt
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
    • C22B7/00—Working up raw materials other than ores, e.g. scrap, to produce non-ferrous metals and compounds thereof; Methods of a general interest or applied to the winning of more than two metals
    • C22B7/005—Separation by a physical processing technique only, e.g. by mechanical breaking
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/54—Reclaiming serviceable parts of waste accumulators
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B09—DISPOSAL OF SOLID WASTE; RECLAMATION OF CONTAMINATED SOIL
    • B09B—DISPOSAL OF SOLID WASTE NOT OTHERWISE PROVIDED FOR
    • B09B2101/00—Type of solid waste
    • B09B2101/15—Electronic waste
    • B09B2101/16—Batteries
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
    • H01M10/0566—Liquid materials
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
    • Y02W30/00—Technologies for solid waste management
    • Y02W30/50—Reuse, recycling or recovery technologies
    • Y02W30/84—Recycling of batteries or fuel cells

Definitions

  • the application relates to a method defined in claim 1 for recycling a battery or batteries and an apparatus defined in claim 12 for recycling a battery or batteries .
  • the most used current process involves possible discharge of the battery and then shredding or grinding of the entire battery cell and separators .
  • the shredded part is known as a black mass which is a combination of different materials , and which also encompasses the active materials , shell casing and polymer materials .
  • the metals are removed either by a magnetic separation or by other filtration process , and the separation of the active material mixture commonly involves the method of flotation where the materials are separated by the hydrophobic and hydrophilic nature of the active materials in cathode and anode . Even though thi s method would be useful , the materials are not fully liberated from each other that has an impact on the purity of the recovered active materials .
  • Document PCT/ JP2020 / 034780 discloses a method for battery material recovery and recycling where the active material is recovered with the help of heating the electrode , which is a resin current collector, to more than the melting part of the resin .
  • the document also discloses a process of flotation .
  • Document WO 2022094169 discloses methods and procedures for repurposing and relithiating the batteries .
  • Document PCT/CN2018 / 119992 discloses a battery manufacturing machine .
  • Document US 20220200042 discloses a method to recover lithium metal from lithium-metal alloys , lithium oxides and lithium feedstock through electrodeposition .
  • Document US 20220029217 discloses a method of extracting the cathode material from the anode and cathode mixture , and it is carried out by a hydrophobicitybased separation process , a filtration separation process based on particle si ze , an eddy current separation and a heat treatment process .
  • Document KR 102201699 discloses a restoration process where the cathode and the anode are disassembled and placed in a restoration solution where the l ithium cations and anions are present .
  • the obj ective is to solve the above problems . Further, the obj ective is to disclose a new-type process for recycling of different batteries and rechargeable batteries . Further, the obj ective is to recycle the batteries effectively . Further, the obj ective is to provide the recycling of the batteries without shredding them . Further, the obj ective is to recover high-quality active materials from the batteries .
  • the method for recycling at least one battery comprising : discharging the battery, dismantling the battery by separating a core of the battery comprising at least one active material from a battery casing, collecting at least one mixture containing the active material from electrodes of the core of the battery, and separating anode and cathode active materials from the mixture for recovering the active materials .
  • the apparatus for recycling at least one battery comprises at least one discharge device to discharge at least one battery, at least one separator device to dismantle a core of the battery comprising at least one active material from a battery casing, at least one collector to collect at least one mixture containing the active material from electrodes of the core , and at least one separation device to separate anode and cathode active materials from the mixture .
  • At least one battery is discharged by treating the battery in an electrolytic bath discharge , the battery is di smantled by separating a core of the battery comprising at least one active material from a battery casing, at least one mixture containing the active material i s collected from electrodes of the core of the battery, and anode and cathode active materials are separated from the mixture for recovering the active materials .
  • the apparatus for recycling at least one battery may comprise at least one electrolytic bath discharge device to discharge at least one battery, at least one separator device comprising a plunger or puller system to separate a core of the battery comprising at least one active material from a battery casing, at least one collector, e . g . vessel or other suitable collector, to collect at least one mixture containing the active material from electrodes of the core , and at least one acoustic separation device to separate anode and cathode active materials from the mixture .
  • the maj or step in the recycling of the batteries is the separation and recovery of the active materials .
  • the separation of the active materials includes the segregation of the anode and cathode materials .
  • the battery means any battery, rechargeable battery, electrochemical cell , or the like .
  • the battery may have any shape .
  • the battery is a cylindrical battery .
  • the battery is a torch battery .
  • the battery is a lithium-ion battery .
  • the battery is a cylindrical lithium-ion cell .
  • the battery is an alkaline cell .
  • the battery is a rechargeable battery.
  • the battery is a solid-state battery.
  • a liquid electrolyte is removed before the separation of the core of the battery from the battery casing.
  • the battery is dismantled by cutting off both ends of the battery casing and by separating the core through the opened ends from the battery casing.
  • the apparatus comprises a cutting device to cut off both ends of the battery casing before the separator device.
  • the cutting device is a laser cutting device.
  • the cutting device may be other suitable cutting device.
  • the core is separated from the battery casing through the opened caps on the battery casing by a mechanical, pneumatical and/or electric push mechanism.
  • the core is separated from the battery casing through the opened caps on the battery casing by a mechanical, pneumatical and/or electric pull mechanism.
  • an electrolyte or electrolytes are removed during the dismantling.
  • the dismantling is carried out essentially in dry conditions, preferably with a relative humidity of less than 20 % .
  • the mixture which contains the active materials is collected from the electrodes of the core of the battery.
  • the mixture may be collected into any suitable collector, e.g. vessel, container, tank, collector, storage bin, or the like.
  • an electrolyte or electrolytes are removed during the collection of the mixture.
  • the collection is carried out in the presence of an acoustic technique and/or chemical reagent (s) .
  • the collection is carried out using an acoustic treatment.
  • the collection of the mixture is carried out in a separate step .
  • the collection of the mixture is carried out j ust before the separation of the active materials or in the the separation step in which the active materials are separated . In one embodiment , the collection of the mixture is carried out in the dismantling step or in the separator device .
  • the separation of the active materials from the mixture can be performed through different methods , in one embodiment by using an acoustic separation method .
  • an electrolyte or electrolytes are removed during the separation of the active materials .
  • the mixture collected from the electrodes is mixed to a fluid, e . g . a carrier fluid, before the separation of the anode and cathode active materials .
  • a fluid e . g . a carrier fluid
  • the acoustic separation is used, and the mixture comprising the active materials is mixed with a carrier fluid that i s chemically inert with the active materials .
  • a ratio of the active material and fluid is less than 10 : 100 .
  • the anode and cathode active materials are separated from the mixture using an acoustic separation, and optionally at least one chemical reagent .
  • the active materials are separated from the mixture using an ultrasonication .
  • the acoustic separation device comprises an ultrasonication device to separate the active materials from the mixture .
  • an indirect ultrasonication treatment is used in the separation .
  • the acoustic separation device comprises a chamber where the anode and cathode active materials are separated from the mixture , and the chamber comprises at least one inlet to feed the mixture and at least two outlets to discharge the active materials .
  • the active material is separated from an electrode sheet .
  • the electrodes are submerged in de-ioni zed water and subj ected to an ultrasonication to remove the active materials .
  • the active material may be any active material , for example the positive electrode may contain metal oxide , lithium-based oxide or the like , e . g . LCO, NCA, NMC, LMO, LMNO, LR-NMC, LFP, or LMFP, and/or the negative electrode may contain graphite , LTO, silicon, or lithium .
  • the positive electrode may contain metal oxide , lithium-based oxide or the like , e . g . LCO, NCA, NMC, LMO, LMNO, LR-NMC, LFP, or LMFP
  • the negative electrode may contain graphite , LTO, silicon, or lithium .
  • the active materials can be divided between the anode and cathode materials .
  • the division of the active materials between the anode and cathode i s based on density or mass dif ference .
  • the active material of the cathode has higher density than the anode material for the efficient functioning of the separation .
  • the active material of the anode has higher density than the cathode material , wherein the difference in the density is at least 1 g/cc ( 1000 kg/m 3 ) .
  • the separation process by the acoustic is not limited to the particular sequence of process steps but can be used in the battery recycling process in which the mass difference exists in the active materials .
  • a heat treatment is used as a pre-process ing step before the separation of the active materials , and the separation is carried by the acoustic force .
  • the collecting of the mixture from the electrodes and/or the separating of the anode and cathode active materials take place in an oxygen-free atmosphere or in an oxygen-depleted atmosphere . Then fire risks associated with the oxidation of the electrolyte in the batteries can be mitigated during the process .
  • the separated active material particles are treated in a further purification process to be reused in the batteries , e . g . lithium-ion batteries .
  • the active material is purified using a filtration .
  • the active material is purified by a filtration using the acoustics .
  • the s i ze of the active material is limited to the maximum si ze of 100 microns .
  • the removal of the active material from the electrodes , along with or without the binder, is performed without breaking the electrode into multiple parts .
  • the method of recycling cylindrical cells comprises the separation of j elly rolls from the batteries , and the collection the active material mixture and the separation of the active materials , as disclosed in this description .
  • the method comprises separating the j elly rolls from the cylindrical cells through the opened caps on the cylindrical cells by a process of mechanical , pneumatical or electric push or a pull mechanism .
  • the batteries can be recycled effectively .
  • cleaner and less energy consuming process for the recovery of the active materials from the battery, e . g . cylindrical battery cells can be provided .
  • the batteries can be recycled without shredding them .
  • the recycling of lithium-ion cells without shredding them can be performed easily and effectively .
  • the acoustic separation is used for recovering the active materials .
  • a melting step which is an uneconomical and expensive process step is not needed in the present invention.
  • the recovery and reclamation of the active materials from the used battery can be performed effectively.
  • the method offers a possibility to recycle the batteries easily, and energy- and cost-effectively.
  • the present invention provides an industrially applicable, simple and affordable way to recycle the different batteries.
  • the method and apparatus is easy and simple to realize in connection with different production processes.
  • Fig. 1 presents the electrolytic bath to discharge the batteries of the residual charge.
  • Fig. 2 presents the battery cap cutter and jelly roll separator machine.
  • Fig. 3 presents a simple representation of the acoustic separation device.
  • the batteries such as cylindrical batteries, is recycled, and an acoustic separation is used.
  • the cylindrical cells are discharged using an electrolytic bath discharge. Ends of the cylindrical cells are cut off without damaging jelly rolls, and the jelly rolls are separated from casings. The separated jelly rolls undergo a separation step, where the active materials and electrolytes are removed, and the separation of the active materials is performed by the non-contact method consisting of ultrasonics treatment, and optionally an addition of a chemical reagent.
  • a black mass that contains the mixture of the active material can be separated by using various techniques, which preferably include an acoustic manipulation technique.
  • the removal of the jelly roll from the battery casing can be performed using the following devices: an eletrolytic bath, and a separator device comprising a laser cutting device, a next part for separating the jelly roll from the casing and collector and separate bins.
  • the electrolytic bath (3) comprising an electrolyte (2) , as presented in Fig. 1, discharges the batteries (1) from the residual charge.
  • Fig. 2 presents the separator device.
  • the laser cutting device (4) cuts both ends of the batteries, and the caps are separated, and the electrolyte if in liquid form is drained in the collector bins (5) .
  • the batteries without the both ends are taken to the next part of device, where a plunger or puller system (7) which may use either a pneumatic force or a fluidic or mechanical force removes the jelly rolls from the casings and the removed jelly rolls are collected in the separate bin(s) (6) .
  • the separator device of Fig. 2 comprises the cutter (4) , such as a laser cutter mechanism, powered by an actuator, motor or the like, which cuts the ends of the batteries, and another actuating mechanism (7) , such as a plunging mechanism, e.g. a pneumatic plunger mechanism, that pushes the jelly rolls into the collector ( 6) .
  • the cutter (4) such as a laser cutter mechanism, powered by an actuator, motor or the like, which cuts the ends of the batteries
  • another actuating mechanism (7) such as a plunging mechanism, e.g. a pneumatic plunger mechanism, that pushes the jelly rolls into the collector ( 6) .
  • the black mass which contains the active material is collected from the jelly rolls.
  • the collection of the black mass is performed without shredding.
  • the collection may comprise acoustic technique and/or chemical reagents.
  • the collected black mass can be separated into anode and cathode active materials using different methods, such as an acoustic manipulation which is describer hereinafter.
  • the collected black mass is treated using an acoustic separation device according to Fig. 3.
  • the collected black mass is mixed to a fluid which preferably, but not limited, have a density greater than the anode active material and less than the cathode active material.
  • the formed fluid (8) is fed into a chamber which has inlets and outlets, e.g. a single channel inlet and a dual channel outlet as presented in Fig. 3.
  • the formed composition of the black mass and the fluid can have the ratio less than 10:100 of the black mass and the fluid.
  • An acoustic transducer (9) emits acoustic waves and a reflector (10) makes standing waves form.
  • the segregated anode and cathode active materials (11) are discharged from the device.
  • the particle size of the active materials should be less than 100 microns to be more efficient in a reuse or in a post-treatment .
  • the active materials of the electrodes were removed from the electrode sheets, i.e. metal foils, using an ultrasonication.
  • the active materials used in the test were LMNO (lithium manganese nickel oxide) and graphite.
  • the process was conducted under atmospheric pressure .

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  • Engineering & Computer Science (AREA)
  • Chemical & Material Sciences (AREA)
  • Materials Engineering (AREA)
  • Manufacturing & Machinery (AREA)
  • Mechanical Engineering (AREA)
  • Organic Chemistry (AREA)
  • Metallurgy (AREA)
  • Environmental & Geological Engineering (AREA)
  • General Life Sciences & Earth Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Geology (AREA)
  • General Chemical & Material Sciences (AREA)
  • Electrochemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Geochemistry & Mineralogy (AREA)
  • Secondary Cells (AREA)

Abstract

La demande concerne un procédé et un appareil de recyclage d'au moins une batterie. La batterie (1) est déchargée par traitement de la batterie dans une décharge de bain électrolytique (3), la batterie est démontée par séparation d'un noyau de la batterie comprenant au moins un matériau actif d'un boîtier de batterie, au moins un mélange contenant le matériau actif est collecté à partir d'électrodes du noyau de la batterie, et des matériaux actifs d'anode et de cathode (11) sont séparés du mélange pour récupérer les matériaux actifs.
PCT/FI2024/050389 2023-07-13 2024-07-11 Procédé et appareil de recyclage de batterie Pending WO2025012520A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
FI20237133 2023-07-13
FI20237133 2023-07-13

Publications (1)

Publication Number Publication Date
WO2025012520A1 true WO2025012520A1 (fr) 2025-01-16

Family

ID=94214769

Family Applications (1)

Application Number Title Priority Date Filing Date
PCT/FI2024/050389 Pending WO2025012520A1 (fr) 2023-07-13 2024-07-11 Procédé et appareil de recyclage de batterie

Country Status (1)

Country Link
WO (1) WO2025012520A1 (fr)

Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN108711651A (zh) * 2018-05-23 2018-10-26 荆门市格林美新材料有限公司 一种废旧电池的资源化回收利用工艺和系统
CN111129632B (zh) * 2019-11-22 2021-07-23 深圳清华大学研究院 废旧三元锂离子电池正负极混合材料回收方法
US20220029217A1 (en) * 2018-11-28 2022-01-27 Li Industries, Inc. Methods and systems for scalable direct recycling of batteries
CN116247321A (zh) * 2023-01-09 2023-06-09 赣州赛可韦尔科技有限公司 一种全组分回收废旧锂离子电池的方法

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN108711651A (zh) * 2018-05-23 2018-10-26 荆门市格林美新材料有限公司 一种废旧电池的资源化回收利用工艺和系统
US20220029217A1 (en) * 2018-11-28 2022-01-27 Li Industries, Inc. Methods and systems for scalable direct recycling of batteries
CN111129632B (zh) * 2019-11-22 2021-07-23 深圳清华大学研究院 废旧三元锂离子电池正负极混合材料回收方法
CN116247321A (zh) * 2023-01-09 2023-06-09 赣州赛可韦尔科技有限公司 一种全组分回收废旧锂离子电池的方法

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