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Recent developments and the future of the recycling of spent graphite for energy storage applications

WANG Ji-rui YANG Da-hai XU Yi-jian HOU Xiang-long EDISON Huixiang Ang WANG De-zhao ZHANG Le ZHU Zhen-dong FENG Xu-yong SONG Xiao-hui XIANG Hong-fa

王继锐, 杨大海, 徐义俭, 侯香龙, EDISONHuixiang Ang, 王德钊, 张乐, 朱振东, 冯绪勇, 宋晓辉, 项宏发. 废旧石墨回收及其储能应用的研究进展. 新型炭材料(中英文), 2023, 38(5): 787-803. doi: 10.1016/S1872-5805(23)60777-2
引用本文: 王继锐, 杨大海, 徐义俭, 侯香龙, EDISONHuixiang Ang, 王德钊, 张乐, 朱振东, 冯绪勇, 宋晓辉, 项宏发. 废旧石墨回收及其储能应用的研究进展. 新型炭材料(中英文), 2023, 38(5): 787-803. doi: 10.1016/S1872-5805(23)60777-2
WANG Ji-rui, YANG Da-hai, XU Yi-jian, HOU Xiang-long, EDISON Huixiang Ang, WANG De-zhao, ZHANG Le, ZHU Zhen-dong, FENG Xu-yong, SONG Xiao-hui, XIANG Hong-fa. Recent developments and the future of the recycling of spent graphite for energy storage applications. New Carbon Mater., 2023, 38(5): 787-803. doi: 10.1016/S1872-5805(23)60777-2
Citation: WANG Ji-rui, YANG Da-hai, XU Yi-jian, HOU Xiang-long, EDISON Huixiang Ang, WANG De-zhao, ZHANG Le, ZHU Zhen-dong, FENG Xu-yong, SONG Xiao-hui, XIANG Hong-fa. Recent developments and the future of the recycling of spent graphite for energy storage applications. New Carbon Mater., 2023, 38(5): 787-803. doi: 10.1016/S1872-5805(23)60777-2

废旧石墨回收及其储能应用的研究进展

doi: 10.1016/S1872-5805(23)60777-2
基金项目: 国家自然科学基金(52072105);安徽省自然科学基金项目(2108085J23、2208085QE134);安徽省属重点研发计划(2021e03020001、202104a05020044);合肥工业大学启动基金(13020-03712021026);新加坡国立教育学院的学术研究基金(RI 1/21 EAH)
详细信息
    通讯作者:

    宋晓辉,副教授. E-mail:xiaohuisong@hfut.edu.cn

    项宏发,教授. E-mail:hfxiang@hfut.edu.cn

  • 中图分类号: 127.1+1

Recent developments and the future of the recycling of spent graphite for energy storage applications

Funds: This work was supported by the National Natural Science Foundation of China (52072105), the Anhui Provincial Natural Science Foundation (2108085J23 and 2208085QE134), Key R&D Program of Anhui Province (2021e03020001 and 202104a05020044), the Start-up grant from Hefei University of Technology (13020-03712021026), and the Academic Research Fund (RI 1/21 EAH) of the National Institute of Education, Singapore
More Information
  • 摘要: 本文对从废旧锂离子电池中获得的电池级石墨的回收和再生进行了广泛的分析。其主要目的是应对供需挑战,最大限度地减少环境污染。该综述主要包括获得、分离、纯化和再生废石墨的方法,以确保其可适用于高质量的储能为目的。为了提高石墨回收效率和去除残留污染物,研究者们探索了热处理、溶剂溶解和超声波处理等技术。本综述进一步评估了湿法和火法冶金的净化和再生方法,考虑了它们对环境的影响和能源消耗等问题。为了可持续和成本效益的提高,可以采用无酸纯化和低温石墨化。讨论了锂离子电池和超级电容器中再生石墨的具体要求,强调了包括酸浸、高温处理和表面涂层在内的回收工艺。这篇综述为开发高效和可持续的储能系统、解决环境问题和满足日益增长的石墨需求提供了宝贵的信息。
  • FIG. 2646.  FIG. 2646.

    FIG. 2646..  FIG. 2646.

    Figure  1.  Failure mechanism of graphite anode electrode in LIBs[40]

    Figure  2.  (a) Recycling technology for spent graphite, (b) Separating electrode plates and active substances to obtain spent graphite. reprinted with permission from Ref.[21], Copyright © 2015 Elsevier Ltd. All rights reserved. (c) Separating cathode and anode electrode active materials to obtain spent graphite. reprinted with permission from Ref.[51], Copyright © 2018, American Chemical Society

    Figure  3.  (a) Flow chart of wet recovery of lithium and spent graphite, (b) Effect of S/L on metal recovery efficiency, (c) Cycle performance of regenerated graphite at room temperature at 1 C. reprinted with permission from Ref.[55], Copyright © 2019 Elsevier Ltd. All rights reserved. (d) Mechanism of graphite regeneration after high-temperature treatment, (e) Cycle stability of PG, HTT-700, HTT-900, HTT-1100, HTT-1300 and HTT-1500 samples under 100 cycles at 1 C. HRTEM images of (f) SG , (g) PG and (h) HTT-900 . reprinted with permission from Ref.[56], Copyright © 2021 Elsevier Ltd. All rights reserved

    Figure  4.  (a) Mechanism diagram of sulfuric acid solidification leaching high temperature calcination reaction, (b) RG spherical aberration electron microscope images, (c) Cycle stability of SG, PG, RG and CG at 0.1 C for 50 cycles. reprinted with permission from Ref.[58] , Copyright © 2020, American Chemical Society. (d) Flash recycling steps for spent batteries. reprinted with permission from Ref.[60], Copyright © 2022 Wiley-VCH GmbH. (e) Schematic diagram of the microwave assisted process for the regeneration and utilization of spent graphite recovered from spent LIBs. reprinted with permission from Ref.[59], Copyright © 2021 Elsevier B.V. All rights reserved

    Figure  5.  (a) Modification methods for fast charging graphite: expanding interlayer spacing, doping, and constructing defects. SEM images of (b) graphite, (c) expanded graphite (EG*) and (d) their thermally annealed version (EG), (e) comparison of interlayer spacing and domain size, (f) magnification performance of graphite, EG * and EG. reprinted with permission from Ref.[65], Copyright © Royal Society of Chemistry

    Figure  6.  (a) Schematic diagram of RG and DRG formation process, HRTEM images of (b) DRG and (c) CG reprinted with permission from Ref.[68], Copyright © 2022, Tsinghua University Press. (d) Schematic diagram of N-RG synthesis, (e) Cyclic performance of CG, SG, and N-RG half cells, (f) Schematic diagram of Li diffusion paths in CG and N-RG. reprinted with permission from Ref.[69], Copyright © 2022 Elsevier Ltd. All rights reserved

    Figure  7.  (a) Na intercalated EG schematic diagram. HRTEM images of (b) PG, (c) GO, (d) EG-1h and (e) EG-5h. reprinted with permission from Ref.[72], Copyright © 2014, Springer Nature Limited. (f) XRD diagram of graphite, (g) point change diagram of the first cycle at 0.1 C, (h) corresponding to the marked XRD pattern in b1. reprinted with permission from Ref.[73], Copyright © 2015, American Chemical Society. (i) XRD images of different temperature heat treatments and RG, and (j) HRTEM images of RG-1300. Cyclic performance of NIB and KIB at (k) 2 A g−1 and (l) 0.2 A g−1, respectively. reprinted with permission from Ref.[75], Copyright ©Royal Society of Chemistry. (m) Structural models of AG and RG, SEM images of (n) AG and (o) RG, cyclic performance of AG at 2000 mA g−1. reprinted with permission from Ref.[76], Copyright © 2020 Elsevier Ltd. All rights reserved

    Figure  8.  (a) Schematic diagram of preparation and working mechanism of Si/SG material, (b, c) HRTEM image of Si/SG, (d) Cycle performance of Si/AG and Si/SG at 1 A g−1 . reprinted with permission from Ref.[80], Copyright © Royal Society of Chemistry. (e) T-SGT/ Si@C Schematic diagram of the synthesis process of anode materials, (f) CGT/ Si@C and T-SGT/ Si@C cyclic performance. reprinted with permission from Ref.[82], Copyright © 2021 Elsevier B.V. All rights reserved. (g) Schematic diagram of adsorption performance and catalytic effect of SG modified separator, (h) Cycle performance of batteries with different separators at 1 C. reprinted with permission from Ref.[85], Copyright © Royal Society of Chemistry

    Table  1.   Recycling methods and high-quality utilization of spent graphite

    MaterialMethodElectrochemical performanceHigh-quality applicationRef.
    Defect-rich recycled graphiteHigh-temperature shock323 mAh g−1 (2 C)Fast-charging graphite material[68]
    N-RGAcid treated, gas-phase exfoliation
    and element doping
    465 mAh g−1 (0.1 A g−1)
    143.5 mAh g−1 (0.4 A g−1)
    Fast-charging graphite material[69]
    Recycled graphitePyrolysis process162 mAh g−1 (0.2 A g−1, SIB)
    320 mAh g−1 (0.05 A g−1, PIB)
    Sodium/potassium battery[75]
    Regeneration graphiteSulfuric acid leaching and High
    temperature heat treatment
    427 mAh g−1 (0.5 C, 200 cycle)
    127 mAh g−1 (50 mA g−1, SIB)
    Sodium/potassium battery[76]
    Si/SG compositeMechanical ball milling1321.8 mAh g−1 (0.05 A g−1)
    69% (1 A g−1, 400 cycle)
    Silicon carbon composite materials[81]
    T-SGT/Si@CHeat treatment, sulfuric acid leaching
    and calcination
    92.47% (500 mA g−1, 300 cycle)
    434.1 mAh g−1 (500 mA g−1)
    Silicon carbon composite materials[82]
    SG-modified separatorSurface coating968 mAh g−1 (1 C)Lithium-sulfur batteries[85]
    CoO/CoFe2O4/EGAcid leaching, high-temperature treatment
    and hydrometallurgy
    890 mAh g−1 (1 A g−1, 700 cycle)
    208 mAh g−1 (5 A g−1)
    High-performance composites materials[29]
    PE/GRx, PP/GRxSolution intercalationComposite separator[86]
    Recovered graphiteUltrasonic peeling and High
    temperature treatment
    185.54 Wh kg−1 (0.319 kW kg−1)
    ~75% (2000 cycle, 10 °C and 25 °C)
    Lithium-ion supercapacitors[90]
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出版历程
  • 收稿日期:  2023-05-31
  • 录用日期:  2023-07-07
  • 修回日期:  2023-07-06
  • 网络出版日期:  2023-08-28
  • 刊出日期:  2023-10-01

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