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Research progress on recovering the components of spent Li-ion batteries

GAO Shao-jun LIU Wei-feng FU Dong-ju LIU Xu-guang

高韶君, 刘伟峰, 符冬菊, 刘旭光. 废旧动力锂离子电池全组分回收技术研究进展. 新型炭材料(中英文), 2022, 37(3): 435-460. doi: 10.1016/S1872-5805(22)60605-X
引用本文: 高韶君, 刘伟峰, 符冬菊, 刘旭光. 废旧动力锂离子电池全组分回收技术研究进展. 新型炭材料(中英文), 2022, 37(3): 435-460. doi: 10.1016/S1872-5805(22)60605-X
GAO Shao-jun, LIU Wei-feng, FU Dong-ju, LIU Xu-guang. Research progress on recovering the components of spent Li-ion batteries. New Carbon Mater., 2022, 37(3): 435-460. doi: 10.1016/S1872-5805(22)60605-X
Citation: GAO Shao-jun, LIU Wei-feng, FU Dong-ju, LIU Xu-guang. Research progress on recovering the components of spent Li-ion batteries. New Carbon Mater., 2022, 37(3): 435-460. doi: 10.1016/S1872-5805(22)60605-X

废旧动力锂离子电池全组分回收技术研究进展

doi: 10.1016/S1872-5805(22)60605-X
基金项目: 国家自然科学基金(51972221,51603142,51902222);山西省重点研发计划国际合作项目 (201903D421077);银川市科技局重点计划项目 (2021ZD08);深圳市科技创新委员会可持续发展项目(KCXFZ20201221173214040);山西省高等学校科技创新项目 (2019L0255,2020L0097)
详细信息
    通讯作者:

    刘伟峰,副教授. E-mail:liuweifeng@tyut.edu.cn

    符冬菊,副主任研究员. E-mail:youyou.orange23@163.com

  • 中图分类号: TQ15

Research progress on recovering the components of spent Li-ion batteries

Funds: All authors acknowledge the financial support by the National Natural Science Foundation of China (51972221, 51603142, 51902222), Key R&D Program of Shanxi Province (International Cooperation, 201903D421077), Key Program of Yinchuan Science and Technology Bureau (2021ZD08), the Sustainable Development Project of the Science and Technology Innovation Commission of Shenzhen (KCXFZ20201221173214040), Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi (2019L0255, 2020L0097)
More Information
  • 摘要: 随着近年来电动汽车的蓬勃发展,锂离子电池的使用量以及退役量都在逐年增长,随之而来的是废旧锂离子电池带来的环境污染以及资源浪费问题。目前商用锂离子电池多由过渡金属氧化物或磷酸盐基正极、石墨基负极、含有害锂盐的有机电解质、聚合物隔膜以及塑料或金属外壳组成,在电池退役后,其中的诸多贵金属以及石墨等都具有较高的回收价值。本文对锂离子电池工作原理及组成结构、废旧锂离子电池全组分回收等研究现状进行了综述,着重介绍废旧锂离子电池中正极材料、负极材料以及电解液回收的研究进展,从回收成本和二次污染等方面概述了不同方法所遇到的问题,最后对未来的发展提供了一些思路。
  • FIG. 1532.  FIG. 1532.

    FIG. 1532.. 

    Figure  1.  (a) Inventory of electric vehicles in various countries in recent years and (b) registered number of electric vehicles in various countries in recent years[7].

    Figure  2.  The components of LIBs and the weight distribution of each part[16] (Reprinted with permission).

    Figure  3.  Charging and discharging working principle of LIBs[18] (Reprinted with permission).

    Figure  4.  (a) Statistics on the contents of each component in spent LIBs[30] (Reprinted with permission) and (b) LIB recycling companies worldwide[25] (Reprinted with permission).

    Figure  5.  Recycling flowchart of spent LIBs.

    Figure  6.  (a) Working principle of the Falcon centrifugal separator[39] (Reprinted with permission). (b) TG-DSC curve of cathode active powder baked at different temperatures[51] (Reprinted with permission). (c) Process of separating positive electrode material and aluminum foil with deep eutectic solvent[56] (Reprinted with permission).

    Figure  7.  (a) Schematic diagram of the leaching mechanism of reducing agent LiFePO4[75] (Reprinted with permission). (b) Comparison of the concentration of inorganic acid and organic acid on the leaching rate of spent LIBs[78] (Reprinted with permission). (c) The influence of the oxalic acid concentration on the reaction efficiency of LiCoO2[49] (Reprinted with permission).

    Figure  8.  (a) Comparison of H2SO4 produced by pH adjustment and without measuring pH change in MS-MC biological leaching system[101] (Reprinted with permission). (b) Metal leaching rates of various strains[102]. (c) Glucosidase oxidation process (Reprinted with permission). (d) Final product leaching efficiencies of precious metals by gluconic acid[103] (Reprinted with permission).

    Figure  9.  The mechanism of ultrasonic cavitation on the leaching process[53] (Reprinted with permission).

    Figure  10.  (a) Preparation process of ion imprinted membrane. (b) Adsorption capacity of ion imprinted membrane for lithium ions at different pH values. (c) Selective adsorption of Li+ by the imprinted membrane[125] (Reprinted with permission).

    Table  1.   Usage of various electric vehicle cathode and anode materials.

    VehicleBattery supplierCathodeAnode
    Renault FluenceAutomotive Energy (Nissan NEC JV)LMOC
    Nissian Leaf EVAutomotive Energy (Nissan NEC JV)LMOC
    Chevrolet VoltCompact Power (subsidiary of LG Chem)LMOC
    BYD E6BYDLFPC
    Tesla Model SPanasonic EnergyNickel-typeC
    Tesla RoadsterPanasonic EnergyNCAC
    Subaru G4eSubaruLVPC
    Honda Fit EVToshiba CorporationNCMLTO
    下载: 导出CSV

    Table  2.   Harmful components in the main components of LIBs and their hazards.

    ComponentHarmful ingredientMain hazard
    Cathode materialHeavy metals such as Co and NiEasily causing dermatitis, respiratory disorder, lung disease,
    and gastrointestinal damage; carcinogenic
    Anode materialCarbon materials such as graphite and acetylene blackThe combustion of the materials produces CO, CO2,
    and other gases and solid dust to pollute the air.
    Lithium salt in electrolyteLiBF4, LiAsF6, LiPF6, etc.Strongly corrosive; it will decompose in water to produce highly
    toxic HF, and produce P2O3 and other toxic substances during
    combustion, which will pollute the environment.
    Electrolyte solventEC, DMC, PC, DMSO, etc.The combustion of the materials produces CO, CO2, and other gases,
    and aldehydes, ketones, and other organic pollutants.
    SeparatorPolypropylene (PP), polyethylene (PE)Naturally difficult to degrade, causing organic pollution
    下载: 导出CSV

    Table  3.   Summary of the research status of leaching spent LIB cathode materials with acids as the leaching agents.

    MaterialsLeaching agentLeaching conditionReduction agentSolid-liquid ratio(g/L)Leaching rateRef.
    LiCoO22 M H2SO480 °C + 1.5 h0.11 M ascorbic acid200Li 95.7%, Co 93.8%[73]
    LiCoO22 M H2SO460 °C + 2 h2% H2O2 (v/v)33Li 87.5%, Co 96.3%[82]
    LiCoO24 M H2SO485 °C + 2 h10% H2O2 (v/v)0.1Li 96%, Co 95%[83]
    LNCM2 M H2SO460 °C + 1 h3% H2O2 (v/v)50Li: 99%; Co: 99%; Ni: 99%; Mn:99%[84]
    LNCM1.5 M H2SO425 °C + 1 h8% H2O2 (v/v)30Li: 80%; Co: 93%; Ni: 92%; Mn:90%[85]
    LNCM0.5 M HNO370 °C +0.15 h0.5 M ascorbic acid20Li, Co, Ni, and Mn~100%[86]
    LiFePO42.5 M H2SO460 °C +4 hN/A100Li: 97%; Fe: 98%[87]
    LiCoO23 M HCl80 °C +40 min3.5% H2O2 (v/v)0.05Li: 81%; Co: 79%[88]
    LiCoO20.7 M H3PO440 °C +1 h4% H2O2 (v/v)50Co: 99.7%; Li: 99.9%[89]
    LiCoO21 M oxalic acid80 °C +2 hN/A50Co, Li: >98%[49]
    LiCoO21.25 M ascorbic acid70 °C +20 minN/A25Co: 94.8%; Li: 98.5%[90]
    LiCoO21.25 M citric acid90 °C +0.5 h1% H2O2 (v/v)16.7Co: 90%; Li: 98%[91]
    LiCoO21.5 M malic acid90 °C +40 min2% H2O2 (v/v)20Co: >90%; Li: ~100%[92]
    LiCoO20.5 M naphthalene disulfonic acid60 °C +0.5 h3% H2O2 (v/v)25Co: 97%; Li: 99%[93]
    LNCM1.2 M DL-malic acid90 °C +0.5 h1.5% H2O2 (v/v)40Li: 98.9%; Co: 94.3%;
    Ni: 95.1%; Mn: 96.4%
    [94]
    LNCM2 M L-Tartaric acid70 °C +0.5 h4% H2O2 (v/v)17Li: 99%; Co: 99%;
    Ni: 99%; Mn: 99%
    [40]
    LNCM0.2 M H3PO4+0.4 M C6H8O790 °C +0.5 hN/A20Li: 100%; Co: 91.63%;
    Ni: 93.38%; Mn: 92%
    [81]
    Note: M: mol L−1
    下载: 导出CSV
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  • 收稿日期:  2022-01-11
  • 修回日期:  2022-02-23
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  • 刊出日期:  2022-06-01

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