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Engineering classification recycling of spent lithium-ion batteries through pretreatment: a comprehensive review from laboratory to scale-up application

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Abstract

The lithium-ion batteries (LIBs) have been widely equipped in electric/hybrid electric vehicles (EVs/HEVs) and the portable electronics due to their excellent electrochemical performances. However, a large number of retired LIBs that consist of toxic substances (e.g., heavy metals, electrolytes) and valuable metals (e.g., Li, Co) will inevitably flow into the waste stream, and their incineration or landfill treatment will cause severe risks to ecosystem and human beings. The sustainable and efficient treatment or recycling of valuable resources from spent LIBs should be fully recognized for environmental and resource security. As one of the most important processes for spent LIBs recycling, the pretreatment is an indispensable step, which is directly related to the subsequent metal extraction and separation processes. Although considerable progresses have been made regarding the pretreatment technologies, there are few summarized reports concerning critical processes of spent LIBs recycling, especially combination of currently available recycling technologies with industrialized applications during pretreatments. Therefore, comprehensive review of the current prevailing pretreatment technologies in laboratory to existing scale-up applications is quite necessary to reveal cutting-edge development in the field of pretreatment. In this review, the current pretreatment technologies are systematically categorized and introduced, along with critical discussions. This review focused on the various options for pretreatment processes itself, instead of general spent LIBs recycling technologies without the focused topics that have been sophisticatedly reviewed by previous studies. Here, the deactivation, discharge, dismantling, separation, liberation of active material and electrolyte treatment have been summarized with the in-depth discussion of the technology development and current status of each category. Finally, current states of industrial development are also reviewed and discussed for the development of efficient and environmentally friendly recycling technologies for future applications. This review tends to present a focused topic concerning the pretreatment of spent LIBs to potential readers with a comprehensive illustration of the development on both cutting-edge technologies and scale-up applications.

Graphical abstract

摘要

锂离子电池（LIBs）由于其出色的电化学性能，已经被广泛地装备在电动/混合电动汽车（EVs/HEVs）和便携式电子产品中。然而，退役LIBs中含有大量的有毒物质（如重金属、电解质）和有价金属（如锂、钴），焚烧或填埋处理将对生态系统和人类造成严重风险。为了环境和资源的安全，可持续和有效地处理或回收废旧LIBs中的宝贵资源是十分重要的。预处理作为废LIBs回收的最重要、不可或缺的过程之一，其好坏直接关系到后续的金属提取和分离过程。尽管在预处理技术方面已经取得了相当大的进展，但有关废旧LIBs回收预处理过程的关键过程的总结却很少，特别是在预处理过程中把目前可用的回收技术与工业化应用相结合。因此，本文全面回顾目前在实验室中流行的预处理技术和现有的放大应用，以揭示预处理领域的前沿发展。在本综述中，对当前的预处理技术进行了系统的分类和介绍，并进行了重要的讨论。本综述侧重于预处理过程的各种方法，而不是介绍一般的废LIBs的回收技术，这在之前的综述中很少见。在这里，总结了失活、放电、拆解、分离、活性材料与集流体的分离和电解质处理等处理技术，并对每一类的技术发展和现状进行了深入讨论。最后，还回顾和讨论了工业发展的现状，以便为未来的应用开发出高效和环保的回收技术。本文倾向于向潜在的读者介绍有关废旧LIBs预处理部分，全面说明前沿技术和放大应用的发展。

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Fig. 1
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Reproduced with permission from Ref. [67]. Copyright 2016, Elsevier. b Change curves and conductivity of different solutions with time and proposed reaction mechanism with conductive solution (Re: electricity percentage). Reproduced with permission from Ref. [62]. Copyright 2016, Elsevier

Fig. 6

Reproduced with permission from Ref. [77]. Copyright 2022, Elsevier. b Sketch of wet impact crusher and particle size distribution of dry or wet crushed products. Reproduced with permission from Ref. [80]. Copyright 2013, Elsevier

Fig. 7

Reproduced with permission from Ref. [11]. Copyright 2022, Elsevier

Fig. 8

Reproduced with permission from Ref. [71]. Copyright 2014, Elsevier. b Particles and aggregates existing in Magnetic-Waterflow separation. Reproduced with permission from Ref. [88]. Copyright 2021, Elsevier. c Sample of granule mixture and corona electrostatic separator (CES) in electrostatic separation. Reproduced with permission from Ref. [91]. Copyright 2020, Sage. d Schematic diagram for graphite and LCO separation using Fenton reagent-assisted flotation. Reproduced with permission from Ref. [100]. Copyright 2017, Elsevier. e Separation diagram of eddy current. Reproduced with permission from Ref. [104]. Copyright 2019, Elsevier. f Schematic of pneumatic separation of spent LIBs in industrial process. Reproduced with permission from Ref. [106]. Copyright 2020, Elsevier

Fig. 9

Reproduced with permission from Ref. [118]. Copyright 2015, Elsevier. b Flowchart for cathode separation by using CaO as heat treatment medium and possible reaction mechanism for PVDF. Reproduced with permission from Ref. [66]. Copyright 2019, ACS. c Separation of active materials from current collectors after pyrolysis. Reproduced with permission from Ref. [123]. Copyright 2016, Elsevier. d Digital pictures of cathode after different treatments under a CO2 atmosphere at 600 °C. Reproduced with permission from Ref. [115]. Copyright 2022, RSC. e Pyrolysis mechanism of cathode at different temperatures. Reproduced with permission from Ref. [125]. Copyright 2022, Elsevier. f Schematic illustration of separating cathode materials and Al foils by low-temperature molten salt (AlCl3-NaCl). Reproduced with permission from Ref. [128]. Copyright 2019, ACS

Fig. 10

Reproduced with permission from Ref. [137]. Copyright 2015, RSC. b Diagram of peeling process and peeling off efficiency by heating ILs ([BMIm][BF4]). Reproduced with permission from Ref. [144]. Copyright 2014, Elsevier. c Schematic of recycling and diagram of DES (choline chloride-ethylene glycol). Reproduced with permission from Ref. [21]. Copyright 2019, Nature. d Schematic of methyl ester solvent synthesis and cathode materials/Al foils separation. Reproduced with permission from Ref. [136]. Copyright 2020, ACS. e Scheme and schematic representation of PVDF dissolution in SC CO2 process. Reproduced with permission from Ref. [154]. Copyright 2021, Elsevier. f Peeling off mechanism with ultrasound-assisted Fenton reaction system. Reproduced with permission from Ref. [135]. Copyright 2021, Elsevier

Fig. 11

Reproduced with permission from Ref. [44]. Copyright 2015, Elsevier. b Mechanism of low-temperature grinding at 77 K. Reproduced with permission from Ref. [162]. Copyright 2019, Elsevier

Fig. 12

Reproduced with permission from Ref. [171]. Copyright 2019, Elsevier. b Schematic illustration of reclaimed electrolytes from spent LIBs. Reproduced with permission from Ref. [178]. Copyright 2017, ACS. c Schematic of low-temperature volatilization. Reproduced with permission from Ref. [23]. Copyright 2020, Elsevier. d Schematic illustration of lab-scale pyrolysis system. Reproduced with permission from Ref. [173]. Copyright 2011, Elsevier

Fig. 13

Reproduced with permission from Ref. [83]. Copyright 2019, Springer. b Schematic diagram of Retriev process. Reproduced with permission from Ref. [11]. Copyright 2021, Elsevier. c Schematic diagram of Accurec process. Reproduced with permission from Ref. [83]. Copyright 2019, Springer

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (Nos. 52074177 and 52174391) and Hunan Provincial Science and Technology Plan, China (No. 2017TP1001). The authors also appreciate the editor(s) and anonymous reviewer(s) with gratitude for their professional comments and constructive suggestions.

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Authors and Affiliations

  1. Hunan Provincial Key Laboratory of Chemical Power Sources, College of Chemistry and Chemical Engineering, Central South University, Changsha, 410083, China

    Shu-Xuan Yan, You-Zhou Jiang & Tao Zhou

  2. College of Chemistry and Chemical Engineering, Hunan Normal University, Changsha, 410083, China

    Xiang-Ping Chen, Lu Yuan & Ting-Ting Min

  3. School of Public Policy and Management, Tsinghua University, Beijing, 100084, China

    Yu Cao

  4. China Nonferrous Metal Industry’s Foreign Engineering and Construction Co., Ltd, Beijing, 100029, China

    Wan-Li Peng

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Yan, SX., Jiang, YZ., Chen, XP. et al. Engineering classification recycling of spent lithium-ion batteries through pretreatment: a comprehensive review from laboratory to scale-up application. Rare Met. 43, 915–941 (2024). https://doi.org/10.1007/s12598-023-02377-y

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