Jiao Lin, Jiawei Wu, Ersha Fan, Xiaodong Zhang, Renjie Chen, Feng Wu,  and Li Li, Environmental and economic assessment of structural repair technologies for spent lithium-ion battery cathode materials, Int. J. Miner. Metall. Mater., 29(2022), No. 5, pp. 942-952. https://doi.org/10.1007/s12613-022-2430-7
Cite this article as:
Jiao Lin, Jiawei Wu, Ersha Fan, Xiaodong Zhang, Renjie Chen, Feng Wu,  and Li Li, Environmental and economic assessment of structural repair technologies for spent lithium-ion battery cathode materials, Int. J. Miner. Metall. Mater., 29(2022), No. 5, pp. 942-952. https://doi.org/10.1007/s12613-022-2430-7
Research Article

Environmental and economic assessment of structural repair technologies for spent lithium-ion battery cathode materials

+ Author Affiliations
  • Corresponding authors:

    Renjie Chen    E-mail: chenrj@bit.edu.cn

    Li Li    E-mail: lily863@bit.edu.cn

  • Received: 10 January 2021Revised: 27 January 2022Accepted: 28 January 2022Available online: 29 January 2022
  • The existing recycling and regeneration technologies have problems, such as poor regeneration effect and low added value of products for lithium (Li)-ion battery cathode materials with a low state of health. In this work, a targeted Li replenishment repair technology is proposed to improve the discharge-specific capacity and cycling stability of the repaired LiCoO2 cathode materials. Compared with the spent cathode material with >50% Li deficiency, the Li/Co molar ratio of the regenerated LiCoO2 cathode is >0.9, which completely removes the Co3O4 impurity phase formed by the decomposition of LixCoO2 in the failed cathode material after repair. The repaired LiCoO2 cathode materials exhibit better cycling stability, lower electrochemical impedance, and faster Li+ diffusion than the commercial materials at both 1 and 10 C. Meanwhile, Li1.05CoO2 cathodes have higher Li replenishment efficiency and cycling stability. The energy consumption and greenhouse gas emissions of LiCoO2 cathodes produced by this repair method are significantly reduced compared to those using pyrometallurgical and hydrometallurgical recycling processes.
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  • [1]
    Y.C. Xue, X.M. Guo, M.R. Wu, J.L. Chen, M.T. Duan, J. Shi, J.H. Zhang, F. Cao, Y.J. Liu, and Q.H. Kong, Zephyranthes-like Co2NiSe4 arrays grown on 3D porous carbon frame-work as electrodes for advanced supercapacitors and sodium-ion batteries, Nano Res., 14(2021), No. 10, p. 3598. doi: 10.1007/s12274-021-3640-4
    [2]
    E.S. Fan, L. Li, Z.P. Wang, J. Lin, Y.X. Huang, Y. Yao, R.J. Chen, and F. Wu, Sustainable recycling technology for Li-ion batteries and beyond: Challenges and future prospects, Chem. Rev., 120(2020), No. 14, p. 7020. doi: 10.1021/acs.chemrev.9b00535
    [3]
    T. Fujita, H. Chen, K.T. Wang, C.L. He, Y.B. Wang, G. Dodbiba, and Y.Z. Wei, Reduction, reuse and recycle of spent Li-ion batteries for automobiles: A review, Int. J. Miner. Metall. Mater., 28(2021), No. 2, p. 179. doi: 10.1007/s12613-020-2127-8
    [4]
    M.R. Wu, M.Y. Gao, S.Y. Zhang, R. Yang, Y.M. Chen, S.Q. Sun, J.F. Xie, X.M. Guo, F. Cao, and J.H. Zhang, High-performance lithium–sulfur battery based on porous N-rich g-C3N4 nanotubes via a self-template method, Int. J. Miner. Metall. Mater., 28(2021), No. 10, p. 1656. doi: 10.1007/s12613-021-2319-x
    [5]
    J. Yang, W.Y. Wang, H.M. Yang, and D.H. Wang, One-pot compositional and structural regeneration of degraded LiCoO2 for directly reusing it as a high-performance lithium-ion battery cathode, Green Chem., 22(2020), No. 19, p. 6489. doi: 10.1039/D0GC02662J
    [6]
    X.P. Fan, C.L. Tan, Y. Li, Z.Q. Chen, Y.H. Li, Y.G. Huang, Q.C. Pan, F.H. Zheng, H.Q. Wang, and Q.Y. Li, A green, efficient, closed-loop direct regeneration technology for reconstructing of the LiNi0.5Co0.2Mn0.3O2 cathode material from spent lithium-ion batteries, J. Hazard. Mater., 410(2021), art. No. 124610. doi: 10.1016/j.jhazmat.2020.124610
    [7]
    MarketsandMarkets, Lithium-ion Battery Recycling Market by Battery Chemistry (Lithium–nickel Manganese Cobalt, Lithium-iron Phosphate, Lithium–Manganese Oxide, LTO, NCA, LCO), Industry (Automotive, Marine, Industrial, and Power), and Region - Global Forecast to 2030 [2021-11-20]. https://www.marketresearch.com/MarketsandMarkets-v3719/Lithium-ion-Battery-Recycling-Chemistry-13018717
    [8]
    J.W. Wu, J. Lin, E.S. Fan, R.J. Chen, F. Wu, and L. Li, Sustainable regeneration of high-performance Li1−xNaxCoO2 from cathode materials in spent lithium-ion batteries, ACS Appl. Energy Mater., 4(2021), No. 3, p. 2607. doi: 10.1021/acsaem.0c03192
    [9]
    S. Gu, L. Zhang, B.T. Fu, J.W. Ahn, and X.P. Wang, Recycling of mixed lithium-ion battery cathode materials with spent lead-acid battery electrolyte with the assistance of thermodynamic simulations, J. Clean. Prod., 266(2020), art. No. 121827. doi: 10.1016/j.jclepro.2020.121827
    [10]
    J. Heelan, E. Gratz, Z.F. Zheng, Q. Wang, M.Y. Chen, D. Apelian, and Y. Wang, Current and prospective Li-ion battery recycling and recovery processes, JOM, 68(2016), No. 10, p. 2632. doi: 10.1007/s11837-016-1994-y
    [11]
    X.L. Zeng, J.H. Li, and L.L. Liu, Solving spent lithium-ion battery problems in China: Opportunities and challenges, Renewable Sustainable Energy Rev., 52(2015), p. 1759. doi: 10.1016/j.rser.2015.08.014
    [12]
    B.L. Zhang, H.W. Xie, B.H. Lu, X. Chen, P.F. Xing, J.K. Qu, Q.S. Song, and H.Y. Yin, A green electrochemical process to recover co and Li from spent LiCoO2-based batteries in molten salts, ACS Sustainable Chem. Eng., 7(2019), No. 15, p. 13391. doi: 10.1021/acssuschemeng.9b02657
    [13]
    J. Lin, E.S. Fan, X.D. Zhang, R.L. Huang, X.X. Zhang, R.J. Chen, F. Wu, and L. Li, A lithium-ion battery recycling technology based on a controllable product morphology and excellent performance, J. Mater. Chem. A, 9(2021), No. 34, p. 18623. doi: 10.1039/D1TA06106B
    [14]
    X.Q. Meng, H.B. Cao, J. Hao, P.G. Ning, G.J. Xu, and Z. Sun, Sustainable preparation of LiNi1/3Co1/3Mn1/3O2–V2O5 cathode materials by recycling waste materials of spent lithium-ion battery and vanadium-bearing slag, ACS Sustainable Chem. Eng., 6(2018), No. 5, p. 5797. doi: 10.1021/acssuschemeng.7b03880
    [15]
    H.J. Bi, H.B. Zhu, L. Zu, Y. Gao, S. Gao, and Y.X. Bai, Environment-friendly technology for recovering cathode materials from spent lithium iron phosphate batteries, Waste Manag. Res., 38(2020), No. 8, p. 911. doi: 10.1177/0734242X20931933
    [16]
    C.R. Borra, J. Mermans, B. Blanpain, Y. Pontikes, K. Binnemans, and T. Van Gerven, Selective recovery of rare earths from bauxite residue by combination of sulfation, roasting and leaching, Miner. Eng., 92(2016), p. 151. doi: 10.1016/j.mineng.2016.03.002
    [17]
    O. Dolotko, I.Z. Hlova, Y. Mudryk, S. Gupta, and V.P. Balema, Mechanochemical recovery of Co and Li from LCO cathode of lithium-ion battery, J. Alloys Compd., 824(2020), art. No. 153876. doi: 10.1016/j.jallcom.2020.153876
    [18]
    H. Dang, N. Li, Z.D. Chang, B.F. Wang, Y.F. Zhan, X. Wu, W.B. Liu, S. Ali, H.D. Li, J.H. Guo, W.J. Li, H.L. Zhou, and C.Y. Sun, Lithium leaching via calcium chloride roasting from simulated pyrometallurgical slag of spent lithium ion battery, Sep. Purif. Technol., 233(2020), art. No. 116025. doi: 10.1016/j.seppur.2019.116025
    [19]
    R.C. Gao, C.H. Sun, L.J. Xu, T. Zhou, L.Q. Zhuang, and H.S. Xie, Recycling LiNi0.5Co0.2Mn0.3O2 material from spent lithium-ion batteries by oxalate co-precipitation, Vacuum, 173(2020), art. No. 109181. doi: 10.1016/j.vacuum.2020.109181
    [20]
    L.Y. Sun, B.R. Liu, T. Wu, G.G. Wang, Q. Huang, Y.F. Su, and F. Wu, Hydrometallurgical recycling of valuable metals from spent lithium-ion batteries by reductive leaching with stannous chloride, Int. J. Miner. Metall. Mater., 28(2021), No. 6, p. 991. doi: 10.1007/s12613-020-2115-z
    [21]
    G. Harper, R. Sommerville, E. Kendrick, L. Driscoll, P. Slater, R. Stolkin, A. Walton, P. Christensen, O. Heidrich, S. Lambert, A. Abbott, K. Ryder, L. Gaines, and P. Anderson, Recycling lithium-ion batteries from electric vehicles, Nature, 575(2019), No. 7781, p. 75. doi: 10.1038/s41586-019-1682-5
    [22]
    C. Yang, J.L. Zhang, Q.K. Jing, Y.B. Liu, Y.Q. Chen, and C.Y. Wang, Recovery and regeneration of LiFePO4 from spent lithium-ion batteries via a novel pretreatment process, Int. J. Miner. Metall. Mater., 28(2021), No. 9, p. 1478. doi: 10.1007/s12613-020-2137-6
    [23]
    Y.J. Liu, Q.Y. Hu, X.H. Li, Z.X. Wang, and H.J. Guo, Recycle and synthesis of LiCoO2 from incisors bound of Li-ion batteries, Trans. Nonferrous Met. Soc. China, 16(2006), No. 4, p. 956. doi: 10.1016/S1003-6326(06)60359-2
    [24]
    J.H. Li, S.W. Zhong, D.L. Xiong, and H. Chen, Synthesis and electrochemical performances of LiCoO2 recycled from the incisors bound of Li-ion batteries, Rare Met., 28(2009), No. 4, p. 328. doi: 10.1007/s12598-009-0064-9
    [25]
    H.H. Nie, L. Xu, D.W. Song, J.S. Song, X.X. Shi, X.Q. Wang, L.Q. Zhang, and Z.H. Yuan, LiCoO2: Recycling from spent batteries and regeneration with solid state synthesis, Green Chem., 17(2015), No. 2, p. 1276. doi: 10.1039/C4GC01951B
    [26]
    X. Song, T. Hu, C. Liang, H.L. Long, L. Zhou, W. Song, L. You, Z.S. Wu, and J.W. Liu, Direct regeneration of cathode materials from spent lithium iron phosphate batteries using a solid phase sintering method, RSC Adv., 7(2017), No. 8, p. 4783. doi: 10.1039/C6RA27210J
    [27]
    Q. Liang, H.F. Yue, S.F. Wang, S.Y. Yang, K.H. Lam, and X.H. Hou, Recycling and crystal regeneration of commercial used LiFePO4 cathode materials, Electrochim. Acta, 330(2020), art. No. 135323. doi: 10.1016/j.electacta.2019.135323
    [28]
    J. Li, Y. Wang, L.H. Wang, B. Liu, and H.M. Zhou, A facile recycling and regeneration process for spent LiFePO4 batteries, J. Mater. Sci. Mater. Electron., 30(2019), No. 15, p. 14580. doi: 10.1007/s10854-019-01830-y
    [29]
    Q.F. Sun, X.L. Li, H.Z. Zhang, D.W. Song, X.X. Shi, J.S. Song, C.L. Li, and L.Q. Zhang, Resynthesizing LiFePO4/C materials from the recycled cathode via a green full-solid route, J. Alloys Compd., 818(2020), art. No. 153292. doi: 10.1016/j.jallcom.2019.153292
    [30]
    Y. Shi, G. Chen, and Z. Chen, Effective regeneration of LiCoO2 from spent lithium-ion batteries: A direct approach towards high-performance active particles, Green Chem., 20(2018), No. 4, p. 851. doi: 10.1039/C7GC02831H
    [31]
    T. Zhang, Y.Q. He, F.F. Wang, H. Li, C.L. Duan, and C.B. Wu, Surface analysis of cobalt-enriched crushed products of spent lithium-ion batteries by X-ray photoelectron spectroscopy, Sep. Purif. Technol., 138(2014), p. 21. doi: 10.1016/j.seppur.2014.09.033
    [32]
    A.T. Appapillai, A.N. Mansour, J. Cho, and Y. Shao-Horn, Microstructure of LiCoO2 with and without “AlPO4” nanoparticle coating: Combined STEM and XPS studies, Chem. Mater., 19(2007), No. 23, p. 5748. doi: 10.1021/cm0715390
    [33]
    Q. Li, K. Wu, M.M. Chen, Y.L. Lee, D.F. Chen, M.M. Wu, F.Q. Li, X.L. Xiao, and Z.B. Hu, Designing high-voltage and high-rate Li1−xNaxCoO2 by enlarging Li layer spacing, Electrochim. Acta, 273(2018), p. 145. doi: 10.1016/j.electacta.2018.04.043
    [34]
    K. Dokko, S. Horikoshi, T. Itoh, M. Nishizawa, M. Mohamedi, and I. Uchida, Microvoltammetry for cathode materials at elevated temperatures: Electrochemical stability of single particles, J. Power Sources, 90(2000), No. 1, p. 109. doi: 10.1016/S0378-7753(00)00456-0
    [35]
    J.W. Qian, L. Liu, J.X. Yang, S.Y. Li, X. Wang, H.L. Zhuang, and Y.Y. Lu, Electrochemical surface passivation of LiCoO2 particles at ultrahigh voltage and its applications in lithium-based batteries, Nat. Commun., 9(2018), art. No. 4918. doi: 10.1038/s41467-018-07296-6
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