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WO2025204167A1 - Procédé et système de traitement de batterie au lithium-ion usagée - Google Patents

Procédé et système de traitement de batterie au lithium-ion usagée

Info

Publication number
WO2025204167A1
WO2025204167A1 PCT/JP2025/003915 JP2025003915W WO2025204167A1 WO 2025204167 A1 WO2025204167 A1 WO 2025204167A1 JP 2025003915 W JP2025003915 W JP 2025003915W WO 2025204167 A1 WO2025204167 A1 WO 2025204167A1
Authority
WO
WIPO (PCT)
Prior art keywords
lithium
aqueous solution
solid
dissolution tank
liquid separation
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/JP2025/003915
Other languages
English (en)
Japanese (ja)
Inventor
弘明 大澤
祥嗣 高田
良介 永井
雅裕 菅田
文典 安藤
晴之 大野
大明 李
峰娃 趙
洋 李
文芳 唐
明俊 宋
静涛 周
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.)
ANHUI CONCH KAWASAKI ENERGY CONSERVATION EQUIPMENT MANUFACTURING Co Ltd
Anhui Conch Kawasaki Energy Conservation Equipment Manufacturing Co Ltd
Kawasaki Heavy Industries Ltd
Kawasaki Motors Ltd
Original Assignee
ANHUI CONCH KAWASAKI ENERGY CONSERVATION EQUIPMENT MANUFACTURING Co Ltd
Anhui Conch Kawasaki Energy Conservation Equipment Manufacturing Co Ltd
Kawasaki Heavy Industries Ltd
Kawasaki Jukogyo KK
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 ANHUI CONCH KAWASAKI ENERGY CONSERVATION EQUIPMENT MANUFACTURING Co Ltd, Anhui Conch Kawasaki Energy Conservation Equipment Manufacturing Co Ltd, Kawasaki Heavy Industries Ltd, Kawasaki Jukogyo KK filed Critical ANHUI CONCH KAWASAKI ENERGY CONSERVATION EQUIPMENT MANUFACTURING Co Ltd
Publication of WO2025204167A1 publication Critical patent/WO2025204167A1/fr
Pending legal-status Critical Current
Anticipated expiration legal-status Critical

Links

Classifications

    • 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
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B09—DISPOSAL OF SOLID WASTE; RECLAMATION OF CONTAMINATED SOIL
    • B09B—DISPOSAL OF SOLID WASTE NOT OTHERWISE PROVIDED FOR
    • B09B5/00—Operations not covered by a single other subclass or by a single other group in this subclass
    • 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
    • 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
    • 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
    • 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
    • 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

  • This disclosure relates to a method and system for processing waste lithium-ion batteries.
  • waste lithium-ion batteries are roasted, and the roasted material is immersed in water to dissolve the lithium ions in the water, separating the lithium from impurities.
  • lithium-ion batteries contain large amounts of fluorine in the electrolyte, binder, etc., and there is a concern that when used lithium-ion batteries are roasted, lithium ions and fluorine ions may combine to produce lithium fluoride. Because lithium fluoride is poorly soluble in water, if it is discarded as residue, the lithium recovery rate will decrease.
  • Patent Document 1 describes adding calcium hydroxide to a lithium solution containing fluorine and lithium in order to separate lithium from the solution.
  • the present disclosure has been made in consideration of the above-mentioned problems, and aims to provide a method and system for processing waste lithium-ion batteries that can promote the dissolution of lithium fluoride and increase the lithium recovery rate.
  • a waste lithium-ion battery treatment system for recovering lithium from waste lithium-ion batteries containing fluorine, and includes: a first dissolving tank into which roasted material obtained by roasting the waste lithium-ion batteries is introduced and immersed in water; a first separator that performs a first solid-liquid separation on the aqueous solution after immersion in the first dissolving tank; a lithium recovery device that recovers the lithium from the aqueous solution separated by the first separator; a second dissolving tank different from the first dissolving tank that introduces and immerses the residue after immersion in the first dissolving tank in water to which calcium hydroxide is added; a second separator that performs a second solid-liquid separation on the aqueous solution after immersion in the second dissolving tank; and a calcium separation device that separates excess calcium derived from the calcium hydroxide and the lithium from the aqueous solution separated by the second solid-liquid separation.
  • the waste LIBs to be treated by the treatment system in this embodiment are, for example, NCM-type lithium-ion batteries, which contain nickel, cobalt, and manganese as the positive electrode active material.
  • NCM-type lithium-ion batteries which contain nickel, cobalt, and manganese as the positive electrode active material.
  • lithium-ion batteries other than NCM-type batteries may also be treated.
  • a lithium-ion battery is a battery that contains graphite as the negative electrode active material, uses aluminum foil as the positive electrode current collector, and copper foil as the negative electrode current collector.
  • a lithium-ion battery contains a fluorine compound as an electrolyte or binder.
  • This processing system targets large waste LIBs, i.e., battery modules made up of multiple waste LIB battery cells, and battery units made up of multiple battery modules.
  • a battery unit for example, is composed of multiple electrically connected battery modules, a control device, and a cooling device housed within a housing.
  • This processing system is intended to remove waste LIBs installed in electric vehicles or hybrid vehicles, for example, and process the removed waste LIBs, i.e., battery units or battery modules, without dismantling them.
  • the processing system in this embodiment includes a thermal decomposition process P1 in which waste LIB is thermally decomposed and the resulting powder containing active material is roasted, and a recovery process P2 in which the roasted active material is immersed in water to elute the lithium, and then the lithium is recovered.
  • the pyrolysis process P1 includes a pretreatment process P11, a crushing and sorting process P12, and a roasting process P13.
  • Figure 2 is a schematic diagram of a pyrolysis system that performs the pyrolysis process shown in Figure 1.
  • the pyrolysis system 1 includes a supply device 10, a pretreatment device 11, a crushing and sorting device 12, and a roasting device 13.
  • the waste LIB is roasted, i.e., pre-roasted, at a second temperature lower than the first temperature in the roasting process P13 described below in order to decompose and remove the electrolyte contained in the waste LIB.
  • the waste LIB is supplied from the supply device 10 to the pre-treatment device 11.
  • the supply device 10 is configured, for example, by a belt conveyor.
  • the pre-treatment device 11 is configured, for example, by a grate preheater.
  • the second temperature in the pretreatment process P11 is set to a temperature at which the electrolyte contained in the waste LIB can be decomposed and removed.
  • the second temperature is equal to or higher than 150°C and lower than 400°C, and may be equal to or higher than 150°C and lower than 250°C.
  • the crushing and sorting process P12 crushes the waste LIBs processed in the pretreatment process P11, and separates the active material from the current collectors of the crushed waste LIBs to sort the active material.
  • the crushing and sorting device 12 is equipped with a crusher 12a and a sorter 12b.
  • the crusher 12a is configured, for example, by a roll crusher.
  • the crusher 12a crushes large waste LIBs (battery units or battery modules) into pieces roughly the size of battery cells or smaller.
  • the sorter 12b is configured to separate the active material from the current collectors of the waste LIB crushed by the crusher 12a, and to sort and extract the active material.
  • the sorter 12b is configured, for example, as a sieve shaker. In reality, the sorter 12b extracts not only the positive electrode active material, but also small amounts of impurities other than the active material, such as the negative electrode active material, and supplies them to the roasting device 13. Other waste LIB packaging materials, current collectors, etc. are sent to separate processing equipment.
  • the waste LIB sorted in the crushing and sorting process P12 is roasted at a predetermined first temperature.
  • the mixed waste LIB is a mixture containing the active material of the waste LIB and an alkali metal salt.
  • the roasting device 13 is, for example, an externally heated rotary kiln.
  • the externally heated rotary kiln has a cylinder 13a that rotates around its central axis and a heating jacket 13b that is arranged to surround the outer periphery of the cylinder 13a.
  • the cylindrical body 13a has an inlet 13c at one end and an outlet 13d at the other end, and is supported so that it can rotate around its central axis with the central axis inclined at a predetermined angle so that it slopes downward from the inlet 13c to the outlet 13d.
  • the waste LIB supplied from the sorter 12b to the inlet 13c of the cylindrical body 13a is transported toward the outlet 13d as the cylindrical body 13a rotates.
  • the interior of the cylinder 13a is an air atmosphere.
  • the interior of the cylinder 13a may be a reducing atmosphere or a low-oxygen atmosphere with an oxygen concentration of, for example, 10% or less.
  • the first temperature which is the roasting temperature in the roasting process P13, is 400°C or higher and may be, for example, 800°C.
  • FIG 3 is a schematic diagram of a recovery system that performs the recovery process shown in Figure 1.
  • Recovery process P2 includes a first dissolution process P21, a first separation process P22, and a lithium recovery process P24.
  • recovery system 2 is equipped with a first dissolution tank 21, a first separator 22, and a lithium recovery device 24.
  • the roasted material is immersed in water.
  • water is stored in the first dissolution tank 21, and the roasted material is introduced into the first dissolution tank 21.
  • the roasted material is supplied to the first dissolution tank 21 in predetermined amounts via a hopper 20.
  • the aqueous solution in the first dissolution tank 21 becomes a mixture of water and the roasted material.
  • the first dissolution tank 21 is equipped with a stirring mechanism that stirs the aqueous solution in the first dissolution tank 21.
  • lithium carbonate Li 2 CO 3
  • the lithium carbonate dissolves in the water in the first dissolution tank 21.
  • the first separation process P22 performs a first solid-liquid separation on the aqueous solution treated in the first dissolution process P21.
  • the first separator 22 is composed of a solid-liquid separator. By performing solid-liquid separation using the first separator 22, solid residue is removed from the aqueous solution.
  • the lithium recovery process P24 recovers lithium from the aqueous solution separated in the first solid-liquid separation.
  • the lithium recovery process P24 concentrates the aqueous solution separated in the first separation process P22.
  • the lithium recovery device 24 may be equipped with a concentrator.
  • the concentrator may be, for example, an evaporation/concentration device or crystallization device that heats the aqueous solution to 80°C or higher and evaporates the water content of the aqueous solution. By concentrating the aqueous solution, the concentration of lithium contained in the aqueous solution increases, and a slurry containing lithium carbonate is produced.
  • the roasted material introduced into the first dissolving tank 21 contains lithium fluoride.
  • waste LIB contains fluorine, which combines with lithium during roasting, etc., to produce lithium fluoride (LiF).
  • Lithium fluoride does not dissolve in water in the first dissolving tank 21 and is contained in the residue.
  • the recovery process P2 includes a second dissolution process P25, a second separation process P26, and a calcium separation process P27.
  • the recovery system 2 is equipped with a second dissolution tank 25, a second separator 26, and a calcium separation device 27.
  • the residue remaining after immersion in the first dissolution tank 21 is introduced into a second dissolution tank 25, which is different from the first dissolution tank 21, and immersed in water.
  • the second dissolution tank 25 is configured to store new water and to receive the residue.
  • the residue is supplied to the second dissolution tank 25 in predetermined amounts via a hopper 30.
  • calcium hydroxide (Ca(OH) 2 ) is added to the water in the second dissolution tank 25.
  • the aqueous solution in the second dissolution tank 25 becomes a mixture of new water, the residue, and calcium hydroxide.
  • the second dissolution tank 25 is equipped with a stirring mechanism for stirring the aqueous solution in the second dissolution tank 25.
  • the second separation process P26 performs a second solid-liquid separation on the aqueous solution treated in the second dissolution process P25.
  • the second separator 26 is composed of a solid-liquid separator.
  • solid residues containing calcium fluoride and other impurities are removed from the aqueous solution.
  • the calcium separation process P27 separates excess calcium derived from calcium hydroxide and lithium from the aqueous solution separated in the second solid-liquid separation.
  • the bubbling with carbon dioxide gas is carried out so that the pH of the aqueous solution separated in the second solid-liquid separation is within the range of 8 to 10. If the pH of the aqueous solution after bubbling is less than 8, the precipitated calcium carbonate may re-dissolve as calcium bicarbonate (Ca(HCO 3 ) 2 ), making it impossible to separate calcium from lithium. Furthermore, since the pH of the aqueous solution before bubbling is around 12, if the pH of the aqueous solution after bubbling is greater than 10, excess calcium cannot be sufficiently precipitated.
  • a processing system is exemplified in which one or more devices or equipment correspond to each process, but the processing system may also be configured to realize multiple processes using one device or equipment.
  • the aqueous solution separated in the calcium separation device 27 was mixed with the aqueous solution separated in the first separator 22 and introduced into the lithium recovery device 24, but these aqueous solutions may also be processed separately.
  • the calcium separation device 27 may have the same function as the lithium recovery device 24, i.e., the function of performing the concentration and solid-liquid separation processes, after the third separation process P29.
  • a method for treating used lithium-ion batteries is a method for recovering lithium from used lithium-ion batteries containing fluorine, the method comprising the steps of: roasting the used lithium-ion batteries to obtain a roasted product, introducing the roasted product into a first dissolving tank and immersing it in water; performing a first solid-liquid separation on the aqueous solution obtained after immersion in the first dissolving tank; recovering the lithium from the aqueous solution separated by the first solid-liquid separation; introducing the residue obtained after immersion in the first dissolving tank into a second dissolving tank different from the first dissolving tank and immersing it in water; adding calcium hydroxide to the water in the second dissolving tank; performing a second solid-liquid separation on the aqueous solution obtained after immersion in the second dissolving tank; and separating excess calcium derived from the calcium hydroxide and the lithium from the aqueous solution separated by the second solid-liquid separation.
  • the roasted product obtained by roasting waste lithium-ion batteries is immersed in water in a first dissolving tank, and the resulting residue is then immersed in water again in a second dissolving tank that is different from the first dissolving tank.
  • calcium hydroxide is added to the second dissolving tank. This promotes the dissolution of lithium fluoride contained in the residue, allowing the lithium contained in the residue to be recovered. This results in a high lithium recovery rate.
  • the weight ratio of the amount of water in the second dissolving tank to the amount of the residue introduced into the second dissolving tank may be 20 to 40 times. This makes it possible to sufficiently dissolve lithium fluoride contained in the residue in the second dissolving tank and to suppress an increase in costs.
  • the aqueous solution separated in the second solid-liquid separation may be bubbled with carbon dioxide gas, and the aqueous solution after the bubbling may be subjected to a third solid-liquid separation to remove the excess calcium as a solid.
  • the excess calcium derived from the calcium hydroxide added in the second dissolution tank can be precipitated. Therefore, lithium and calcium contained in the aqueous solution separated in the second solid-liquid separation can be easily separated. This makes it possible to prevent the purity of the recovered lithium carbonate from being reduced by the added calcium.
  • the bubbling with carbon dioxide gas may be carried out so that the pH of the aqueous solution separated in the second solid-liquid separation falls within a range of 8 to 10. This allows calcium in the aqueous solution to be appropriately separated from lithium.
  • a treatment system for waste lithium-ion batteries is a treatment system for waste lithium-ion batteries for recovering lithium from waste lithium-ion batteries containing fluorine, the treatment system including: a first dissolving tank into which a roasted product obtained by roasting the waste lithium-ion batteries is introduced and immersed in water; a first separator that performs a first solid-liquid separation on the aqueous solution after immersion in the first dissolving tank; a lithium recovery device that recovers the lithium from the aqueous solution separated by the first separator; a second dissolving tank different from the first dissolving tank, into which a residue after immersion in the first dissolving tank is introduced and immersed in water to which calcium hydroxide is added; a second separator that performs a second solid-liquid separation on the aqueous solution after immersion in the second dissolving tank; and a calcium separation device that separates excess calcium derived from the calcium hydroxide and the lithium from the aqueous solution separated by the

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

Abstract

La présente invention concerne un procédé de traitement d'une batterie au lithium-ion usagée pour récupérer le lithium à partir d'une batterie au lithium-ion usagée qui contient du fluor consistant à : introduire un matériau grillé qui est obtenu en grillant la batterie au lithium-ion usagée dans un premier réservoir de dissolution de façon à immerger le matériau grillé dans de l'eau ; réaliser une première séparation solide-liquide sur la solution aqueuse après immersion dans le premier réservoir de dissolution ; récupérer le lithium à partir de la solution aqueuse qui est séparée par la première séparation solide-liquide ; introduire le résidu après immersion dans le premier réservoir de dissolution dans un second réservoir de dissolution, qui est différent du premier réservoir de dissolution, de façon à immerger le résidu dans l'eau ; ajouter de l'hydroxyde de calcium à l'eau dans le second réservoir de dissolution ; réaliser une seconde séparation solide-liquide sur la solution aqueuse après immersion dans le second réservoir de dissolution ; et séparer le calcium en excès, qui est dérivé de l'hydroxyde de calcium, et le lithium de la solution aqueuse qui est séparé par la seconde séparation solide-liquide.
PCT/JP2025/003915 2024-03-28 2025-02-06 Procédé et système de traitement de batterie au lithium-ion usagée Pending WO2025204167A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
CN202410372342.X 2024-03-28
CN202410372342.XA CN120728055A (zh) 2024-03-28 2024-03-28 废锂离子电池的处理方法和处理系统

Publications (1)

Publication Number Publication Date
WO2025204167A1 true WO2025204167A1 (fr) 2025-10-02

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PCT/JP2025/003915 Pending WO2025204167A1 (fr) 2024-03-28 2025-02-06 Procédé et système de traitement de batterie au lithium-ion usagée

Country Status (2)

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CN (1) CN120728055A (fr)
WO (1) WO2025204167A1 (fr)

Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN111635999A (zh) * 2020-06-08 2020-09-08 孟元 一种含锂卤水中提取锂并制备氢氧化锂的方法
WO2020246079A1 (fr) * 2019-06-07 2020-12-10 川崎重工業株式会社 Système et procédé de traitement de batterie au lithium-ion usée
WO2021090571A1 (fr) * 2019-11-08 2021-05-14 Ｄｏｗａエコシステム株式会社 Procédé de séparation du lithium
JP2023106309A (ja) * 2022-01-20 2023-08-01 Ｄｏｗａエコシステム株式会社 有価物の回収方法
JP2023129361A (ja) * 2022-03-03 2023-09-14 三菱マテリアル株式会社 リチウム濃縮液の製造方法及びこれに用いるリン酸リチウムの生成方法

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2020246079A1 (fr) * 2019-06-07 2020-12-10 川崎重工業株式会社 Système et procédé de traitement de batterie au lithium-ion usée
WO2021090571A1 (fr) * 2019-11-08 2021-05-14 Ｄｏｗａエコシステム株式会社 Procédé de séparation du lithium
CN111635999A (zh) * 2020-06-08 2020-09-08 孟元 一种含锂卤水中提取锂并制备氢氧化锂的方法
JP2023106309A (ja) * 2022-01-20 2023-08-01 Ｄｏｗａエコシステム株式会社 有価物の回収方法
JP2023129361A (ja) * 2022-03-03 2023-09-14 三菱マテリアル株式会社 リチウム濃縮液の製造方法及びこれに用いるリン酸リチウムの生成方法

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