| Citation: |
Shuo-Hang Zheng, Xiao-Tong Wang, Zhen-Yi Gu, Jin-Zhi Guo, Xing-Long Wu, et al. Advances and Challenges on Recycling the Electrode and Electrolyte Materials in Spent Lithium-Ion Batteries. Materials Lab 2022, 1, 220036. doi: 10.54227/mlab.20220036
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Advances and Challenges on Recycling the Electrode and Electrolyte Materials in Spent Lithium-Ion Batteries
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Abstract
Lithium-ion batteries (LIBs), as the advanced power batteries with comprehensive performance, have widely used in electric vehicles (EVs), military equipment, aerospace, consumer electronics, and other fields. With the surge in demand for LIBs, the number of spent LIBs has increased rapidly. However, if the spent LIBs just are simply landfilled, the hazardous components contained in them such as heavy metals and organic electrolytes will pollute the environment, and ultimately threaten human health. In addition, some valuable components will be wasted by landfill, especially high-value metal elements contained in cathode. Thus, the recycling of spent LIBs is a "two birds with one stone" strategy which is not only beneficial to environmental protection but also has high economic value. Accordingly, great efforts have been made to develop efficient and cost-effective recycling processes for spent LIBs recovery. In line with the recycling process, this review first presents a series of pretreatment progresses (disassembling, inactivation, dismantling, and separation) and discusses the problems and challenges involved (automation, environmental protection, and cost, etc.). Second, we summarize and discuss the current recovery and regeneration technologies for cathode materials, including pyrometallurgy, hydrometallurgy and electrochemistry. In addition, advances in the recovery of anode and electrolyte are also introduced. Finally, based on the current state of recycling, we cautiously make some suggestions and prospects for the future recycling of spent LIBs, with a view to providing more ideas for the recycling of used LIBs.
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Author Biographies
Shuo-Hang Zheng received his bachelor’s degree from Hebei University of Science and Technology in 2013. He received his master’s degree from Nanjing Tech University. He is currently pursuing his doctorate under the supervise of Professor Xing-Long Wu of Northeast Normal University. He mainly focuses on the recycling and utilization of spent Li-ion batteries. 
Xing-Long Wu is currently a Professor of Chemistry at Northeast Normal University, China. He received his Ph.D. from Institute of Chemistry, Chinese Academy of Sciences (ICCAS) in 2011. After continuing a two-years postdoctoral working in ICCAS, he moved to Northeast Normal University as an Associate Professor in 2013, and become Full Professor in 2018. His current research interests focus on the advanced materials for energy storage devices such as Na/K/Li-ion batteries and dual-ion batteries, and the reuse and recycle of spent LIBs. 
Hai-Yang Xu received his Ph.D. degree from the Changchun Institute of Optics, Fine Mechanics and Physics, Chinese Academy of Science, in 2006. During 2006–2008, he worked as a postdoctoral fellow in the Chinese University of Hong Kong. Currently, he is a professor at the Key Laboratory of UV-Emitting Materials and Technology, Ministry of Education, Northeast Normal University. His research interests include wide-bandgap semiconductor materials and their photonic/electronic devices, memristive materials and devices, and artificial synaptics. -
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Shuo-Hang Zheng, Xiao-Tong Wang, Zhen-Yi Gu, Jin-Zhi Guo, Xing-Long Wu, et al. Advances and Challenges on Recycling the Electrode and Electrolyte Materials in Spent Lithium-Ion Batteries. Materials Lab 2022, 1, 220036. doi: 10.54227/mlab.20220036
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Figure 1.
Distribution of mining production for LIB materials in 2020.[7]
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Figure 2.
Flowchart of the typical processes for spent LIBs recovery.
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Figure 3.
Flowchart of the pretreatment for spent LIBs: Disassembling,[8-12] Inactivation,[13-15] Dismantling,[16] and Separation.[17, 18] Copyright 2021, MDPI.[8] Copyright 2015, Elsevier.[9] Copyright 2014, Trans Tech Publications.[10] Copyright 2018, Elsevier.[11] Copyright 2018, John Wiley & Sons, Ltd.[12] Copyright 2020, Elsevier.[13] Copyright 2020, Elsevier.[16] Copyright 2021, Elsevier.[18]
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Figure 4.
Equipment for different disassembling processes: (a) Pneumatic tool for manual disassembling process.[12] Copyright 2018, John Wiley & Sons, Ltd. (b) Electric screwdriver for semi-automatic disassembling.[9] Copyright 2015, Elsevier. (c) Concept for a disassembly system.[19] Copyright 2021, Elsevier. (d) Task planner for automatic process.[8] Copyright 2021, MDPI.
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Figure 5.
Development of hydrometallurgical and pyrometallurgical processes for spent LIBs recovery. Hydrometallurgical process includes inorganic acid (H2SO4,[32] HCl[33]), reducing agent,[34] organic acid,[35] bioleaching,[36] alkali,[37] subcritical water,[38] and DES[39]. Pyrometallurgical process includes smelting[40] and roasting[41] (sulfation roasting,[42] graphite,[43] and molten salt[44]). Copyright 1989, The Society of Chemical Engineers, Japan.[32] Copyright 1998, Elsevier.[33] Copyright 2001, The Korean Institute of Resources Recycling.[34] Copyright 2010, Elsevier.[35] Copyright 2008, Elsevier.[36] Copyright 2016, Elsevier.[37, 38] Copyright 2019, Springer Nature.[39] Copyright 2007, CNKI.[40] Copyright 2006, Elsevier.[41] Copyright 2011, CNKI.[42] Copyright 2016, Elsevier.[43] Copyright 2019, American Chemical Society.[44]
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Figure 6.
Illustration of the different separation process: (a) Solvent extraction.[89] Copyright 2021, American Chemical Society. (b) Chemical precipitation.[90] Copyright 2016, Elsevier. (c) Electrolysis.[91] Copyright 2021, Elsevier.
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Figure 7.
Flowchart of regeneration process for cathode materials: (a) Hydrothermal method.[107] Copyright 2020, American Chemical Society. (b) Solid phase method.[110] Copyright 2021, Elsevier. (c) Co-precipitation.[98] Copyright 2017, Elsevier. (d) Sol-gel method.[118] Copyright 2017, American Chemical Society.
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Figure 8.
(a) The flowchart of the 3D sea-urchin-like CoN-Gr-2 preparation process from spent LIBs, and the enhanced water splitting performance of CoN-Gr-2.[130] Copyright 2021, Elsevier. (b) Schematic diagram of modified separator by spent LiCoO2 cathode.[133] Copyright 2020, American Chemical Society (c) Using of spent LiCoO2 to regulate the π-conjugated structure of g-C3N4 and the mechanism of synergistic effect of Li-Cl-Co.[131] Copyright 2021, The Royal Society of Chemistry.
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Figure 9.
(a) Preparation of 2D graphene oxide by graphite in spent LIBs.[135] Copyright 2021, Elsevier. (b) Regeneration of the anode.[136] Copyright 2019, Elsevier. (c) Preparation of ORR catalyst by he spent graphite anode.[137] Copyright 2021, Wiley-VCH GmbH. (d) Spent graphite anode used as electrode materials for dual-ion battery.[138] Copyright 2022, Springer Nature.
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Figure 10.
(a) Thermolysis of battery electrolyte produced syngas.[149] Copyright 2021, Elsevier. (b) Reclaimed electrolytes from spent LIBs.[150] Copyright 2017, American Chemical Society.
