Miao Du, Hongyan Lü, Kaidi Du, Shuohang Zheng, Xiaotong Wang, Xiaotong Deng, Ronghua Zeng,  and Xinglong Wu, Upcycling the spent graphite/LiCoO2 batteries for high-voltage graphite/LiCoPO4-co-workable dual-ion batteries, Int. J. Miner. Metall. Mater., 31(2024), No. 7, pp. 1745-1751. https://doi.org/10.1007/s12613-023-2807-2
Cite this article as:
Miao Du, Hongyan Lü, Kaidi Du, Shuohang Zheng, Xiaotong Wang, Xiaotong Deng, Ronghua Zeng,  and Xinglong Wu, Upcycling the spent graphite/LiCoO2 batteries for high-voltage graphite/LiCoPO4-co-workable dual-ion batteries, Int. J. Miner. Metall. Mater., 31(2024), No. 7, pp. 1745-1751. https://doi.org/10.1007/s12613-023-2807-2
Research Article

Upcycling the spent graphite/LiCoO2 batteries for high-voltage graphite/LiCoPO4-co-workable dual-ion batteries

+ Author Affiliations
  • Corresponding author:

    Xinglong Wu    E-mail: xinglong@nenu.edu.cn

  • Received: 18 October 2023Revised: 23 November 2023Accepted: 5 December 2023Available online: 8 December 2023
  • The worldwide proliferation of portable electronics has resulted in a dramatic increase in the number of spent lithium-ion batteries (LIBs). However, traditional recycling methods still have limitations because of such huge amounts of spent LIBs. Therefore, we proposed an ecofriendly and sustainable double recycling strategy to concurrently reuse the cathode (LiCoO2) and anode (graphite) materials of spent LIBs and recycled LiCoPO4/graphite (RLCPG) in $ {\text{L}\text{i}}^{+}/{{\text{P}\text{F}}}_{6}^{-} $ co-de/intercalation dual-ion batteries. The recycle-derived dual-ion batteries of Li/RLCPG show impressive electrochemical performance, with an appropriate discharge capacity of 86.2 mAh·g−1 at 25 mA·g−1 and 69% capacity retention after 400 cycles. Dual recycling of the cathode and anode from spent LIBs avoids wastage of resources and yields cathode materials with excellent performance, thereby offering an ecofriendly and sustainable way to design novel secondary batteries.
  • loading
  • Supplementary Information-s12613-023-2807-2.docx
  • [1]
    P.K. Jones, U. Stimming, and A.A. Lee, Impedance-based forecasting of lithium-ion battery performance amid uneven usage, Nat. Commun., 13(2022), No. 1, art. No. 4806. doi: 10.1038/s41467-022-32422-w
    [2]
    Z.Y. Gu, J.Z. Guo, J.M. Cao, et al., An advanced high-entropy fluorophosphate cathode for sodium-ion batteries with increased working voltage and energy density, Adv. Mater., 34(2022), No. 14, art. No. 2110108. doi: 10.1002/adma.202110108
    [3]
    Q.P. Lu, Z.H. Du, J. Wang, et al., Editorial for special issue on renewable energy conversion, utilization and storage, Int. J. Miner. Metall. Mater., 30(2023), No. 10, p. 1855. doi: 10.1007/s12613-023-2746-y
    [4]
    Z.Z. Yu, G.Q. Zhao, F.L. Ji, et al., Collaboratively enhancing electrochemical properties of LiNi0.83Co0.11Mn0.06O2 through doping and coating of quadrivalent elements, Rare Met., 42(2023), No. 12, p. 4103. doi: 10.1007/s12598-023-02356-3
    [5]
    R. Zhang, C.Y. Wang, P.C. Zou, et al., Compositionally complex doping for zero-strain zero-cobalt layered cathodes, Nature, 610(2022), No. 7930, p. 67. doi: 10.1038/s41586-022-05115-z
    [6]
    J. Lin, E.S. Fan, X.D. Zhang, et al., Sustainable upcycling of spent lithium-ion batteries cathode materials: Stabilization by in situ Li/Mn disorder, Adv. Energy Mater., 12(2022), No. 26, art. No. 2201174. doi: 10.1002/aenm.202201174
    [7]
    K. Kim, D. Raymond, R. Candeago, and X. Su, Selective cobalt and nickel electrodeposition for lithium-ion battery recycling through integrated electrolyte and interface control, Nat. Commun., 12(2021), No. 1, art. No. 6554. doi: 10.1038/s41467-021-26814-7
    [8]
    M. Du, J.Z. Guo, S.H. Zheng, et al., Direct reuse of LiFePO4 cathode materials from spent lithium-ion batteries: Extracting Li from brine, Chin. Chem. Lett., 34(2023), No. 6, art. No. 107706. doi: 10.1016/j.cclet.2022.07.049
    [9]
    K.Y. Zhang, Y.Z. Xu, Y.C. Lin, et al., Enriching redox active sites by interconnected nanowalls-like nickel cobalt phospho-sulfide nanosheets for high performance supercapacitors, Chin. Chem. Lett., 32(2021), No. 11, p. 3553. doi: 10.1016/j.cclet.2021.02.034
    [10]
    Y.T. Xu, S.J. Dai, X.F. Wang, X.W. Wu, Y.G. Guo, and X.X. Zeng, An ion-percolating electrolyte membrane for ultrahigh efficient and dendrite-free lithium metal batteries, InfoMat, 5(2023), No. 12, art. No. e12498. doi: 10.1002/inf2.12498
    [11]
    J.J. Roy, S. Rarotra, V. Krikstolaityte, et al., Green recycling methods to treat lithium-ion batteries e-waste: A circular approach to sustainability, Adv. Mater., 34(2022), No. 25, art. No. 2103346. doi: 10.1002/adma.202103346
    [12]
    M. Xiang, W.X. Fan, W. Lin, et al., Triple kill: Fabrication of composites coming from waste face masks, polystyrene microplastics, graphene, and their electromagnetic interference shielding behaviors, Carbon Neutralization, 2(2023), No. 5, p. 616. doi: 10.1002/cnl2.86
    [13]
    K.D. Du, E.H. Ang, X.L. Wu, and Y.C. Liu, Progresses in sustainable recycling technology of spent lithium-ion batteries, Energy Environ. Mater., 5(2022), No. 4, p. 1012. doi: 10.1002/eem2.12271
    [14]
    J. Wang, Y.F. Yuan, X.H. Rao, et al., Realizing high-performance Na3V2(PO4)2O2F cathode for sodium-ion batteries via Nb-doping, Int. J. Miner. Metall. Mater., 30(2023), No. 10, p. 1859. doi: 10.1007/s12613-023-2666-x
    [15]
    Y.N. Yang, Y.J. Yang, C.L. He, et al., Solvent extraction and separation of cobalt from leachate of spent lithium-ion battery cathodes with N263 in nitrite media, Int. J. Miner. Metall. Mater., 30(2023), No. 5, p. 897. doi: 10.1007/s12613-022-2571-8
    [16]
    H.Y. Lu, R.L. Hou, S.Y. Chu, H.S. Zhou, and S.H. Guo, Progress on modification strategies of layered lithium-rich cathode materials for high energy lithium-ion batteries, Acta Phys. Chim. Sin., 39(2023), No. 7, art. No. 2211057.
    [17]
    Z.J. Baum, R.E. Bird, X. Yu, and J. Ma, Lithium-ion battery recycling─Overview of techniques and trends, ACS Energy Lett., 7(2022), No. 2, p. 712. doi: 10.1021/acsenergylett.1c02602
    [18]
    C.M. Costa, J.C. Barbosa, R. Gonçalves, H. Castro, F.J. del Campo, and S. Lanceros-Méndez, Recycling and environmental issues of lithium-ion batteries: Advances, challenges and opportunities, Energy Storage Mater., 37(2021), p. 433. doi: 10.1016/j.ensm.2021.02.032
    [19]
    M. Wasesa, T. Hidayat, D.T. Andariesta, et al., Economic and environmental assessments of an integrated lithium-ion battery waste recycling supply chain: A hybrid simulation approach, J. Clean. Prod., 379(2022), art. No. 134625. doi: 10.1016/j.jclepro.2022.134625
    [20]
    R.C. Xu, L.H. Jiang, N. Duan, et al., Research on microstructure of membrane-slime layer on lead-based anode surface in zinc hydrometallurgy by combining μ-XRF with mm-XRF, J. Clean. Prod., 379(2022), art. No. 134568. doi: 10.1016/j.jclepro.2022.134568
    [21]
    X.T. Wang, Z.Y. Gu, E.H. Ang, X.X. Zhao, X.L. Wu, and Y.C. Liu, Prospects for managing end-of-life lithium-ion batteries: Present and future, Interdiscip. Mater., 1(2022), No. 3, p. 417. doi: 10.1002/idm2.12041
    [22]
    T. Zhong, H.Y. Zhang, M.C. Song, et al., FeCoNiCrMo high entropy alloy nanosheets catalyzed magnesium hydride for solid-state hydrogen storage, Int. J. Miner. Metall. Mater., 30(2023), No. 11, p. 2270. doi: 10.1007/s12613-023-2669-7
    [23]
    Y.L. Heng, Z.Y. Gu, J.Z. Guo, and X.L. Wu, Research progresses on vanadium-based cathode materials for aqueous zinc-ion batteries, Acta Phys. Chim. Sin., 37(2021), No. 3, art. No. 2005013.
    [24]
    L. Cassayre, B. Guzhov, M. Zielinski, and B. Biscans, Chemical processes for the recovery of valuable metals from spent nickel metal hydride batteries: A review, Renewable Sustainable Energy Rev., 170(2022), art. No. 112983. doi: 10.1016/j.rser.2022.112983
    [25]
    Y.H. Miao, S.Y. Qi, G. Chen, et al., Efficient removal of As, Cu and Cd and synthesis of photo-catalyst from Cu-smelting waste acid through sulfide precipitation by biogenic gaseous H2S produced by anaerobic membrane bioreactor, Chem. Eng. J., 451(2023), art. No. 138096. doi: 10.1016/j.cej.2022.138096
    [26]
    H. Dang, Z.D. Chang, H.L. Zhou, S.H. Ma, M. Li, and J.L. Xiang, Extraction of lithium from the simulated pyrometallurgical slag of spent lithium-ion batteries by binary eutectic molten carbonates, Int. J. Miner. Metall. Mater., 29(2022), No. 9, p.1715. doi: 10.1007/s12613-021-2366-3
    [27]
    K.D. Du, Y.F. Meng, X.X. Zhao, et al., A unique co-recovery strategy of cathode and anode from spent LiFePO4 battery, Sci. China Mater., 65(2022), No. 3, p. 637. doi: 10.1007/s40843-021-1772-6
    [28]
    J. Lin, J.W. Wu, E.S. Fan, et al., Environmental and economic assessment of structural repair technologies for spent lithium-ion battery cathode materials, Int. J. Miner. Metall. Mater., 29(2022), No. 5, p. 942. doi: 10.1007/s12613-022-2430-7
    [29]
    T. Wang, H.M. Luo, Y.C. Bai, J.L. Li, I. Belharouak, and S. Dai, Direct recycling of spent NCM cathodes through ionothermal lithiation, Adv. Energy Mater., 10(2020), No. 30, art. No. 2001204. doi: 10.1002/aenm.202001204
    [30]
    B. Xu, P. Dong, J.G. Duan, D. Wang, X.S. Huang, and Y.J. Zhang, Regenerating the used LiFePO4 to high performance cathode via mechanochemical activation assisted V5+ doping, Ceram. Int., 45(2019), No. 9, p. 11792. doi: 10.1016/j.ceramint.2019.03.057
    [31]
    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
    [32]
    S.H. Zheng, X.T. Wang, Z.Y. Gu, J.Z. Guo, X.L. Wu, and H.Y. Xu, Advances and challenges on recycling the electrode and electrolyte materials in spent lithium-ion batteries, Mater. Lab, 1(2022), No. 4, art. No. 220036. doi: 10.54227/mlab.20220036
    [33]
    Z.Y. Gu, J.Z. Guo, X.X. Zhao, et al., High-ionicity fluorophosphate lattice via aliovalent substitution as advanced cathode materials in sodium-ion batteries, InfoMat, 3(2021), No. 6, p. 694. doi: 10.1002/inf2.12184
    [34]
    M.C. Guo, W. Tang, Y. Hong, et al., Self-carbonization of soluble organic cathodes enables stable Na-ion batteries, Sci. China Mater., 66(2023), No. 7, p. 2621. doi: 10.1007/s40843-022-2405-6
    [35]
    Y. Yang, J.Z. Guo, Z.Y. Gu, et al., Effective recycling of the whole cathode in spent lithium ion batteries: From the widely used oxides to high-energy/stable phosphates, ACS Sustainable Chem. Eng., 7(2019), No. 14, p. 12014. doi: 10.1021/acssuschemeng.9b00526
    [36]
    M. Du, K.D. Du, J.Z. Guo, et al., Direct reuse of oxide scrap from retired lithium-ion batteries: Advanced cathode materials for sodium-ion batteries, Rare Met., 42(2023), No. 5, p. 1603. doi: 10.1007/s12598-022-02230-8
    [37]
    J.L. Yang, X.X. Zhao, W.H. Li, et al., Advanced cathode for dual-ion batteries: Waste-to-wealth reuse of spent graphite from lithium-ion batteries, eScience, 2(2022), No. 1, p. 95. doi: 10.1016/j.esci.2021.11.001
    [38]
    K.K. Jena, A. AlFantazi, and A.T. Mayyas, Efficient and cost-effective hybrid composite materials based on thermoplastic polymer and recycled graphite, Chem. Eng. J., 430(2022), art. No. 132667. doi: 10.1016/j.cej.2021.132667
    [39]
    Y.F. Meng, H.J. Liang, C.D. Zhao, et al., Concurrent recycling chemistry for cathode/anode in spent graphite/LiFePO4 batteries: Designing a unique cation/anion-co-workable dual-ion battery, J. Energy Chem., 64(2022), p. 166. doi: 10.1016/j.jechem.2021.04.047
    [40]
    N.J. Zhang, W.J. Deng, Z.X. Xu, and X.L. Wang, Upcycling of spent LiCoO2 cathodes via nickel- and manganese-doping, Carbon Energy, 5(2023), No. 1, art. No. e231. doi: 10.1002/cey2.231
    [41]
    J.X. Zhang, P.F. Wang, P.X. Bai, et al., Interfacial design for a 4.6 V high-voltage single-crystalline LiCoO2 cathode, Adv. Mater., 34(2022), No. 8, art. No. 2108353. doi: 10.1002/adma.202108353
    [42]
    J.Z. Guo, H.X. Zhang, Z.Y. Gu, et al., Heterogeneous NASICON-type composite as low-cost, high-performance cathode for sodium-ion batteries, Adv. Funct. Mater., 32(2022), No. 52, art. No. 2209482. doi: 10.1002/adfm.202209482
    [43]
    J.Y. Wu and C.J. Tsai, Qualitative modeling of the electrolyte oxidation in long-term cycling of LiCoPO4 for high-voltage lithium-ion batteries, Electrochim. Acta, 368(2021), art. No. 137585. doi: 10.1016/j.electacta.2020.137585
    [44]
    N. Priyadharsini, S. Shanmugapriya, P.R. Kasturi, S. Surendran, and R.K. Selvan, Morphology-dependent electrochemical properties of sol-gel synthesized LiCoPO4 for aqueous hybrid capacitors, Electrochim. Acta, 289(2018), p. 516. doi: 10.1016/j.electacta.2018.08.086
    [45]
    Y. Wang, J.Y. Qiu, Z.B. Yu, et al., AlF3-modified LiCoPO4 for an advanced cathode towards high energy lithium-ion battery, Ceram. Int., 44(2018), No. 2, p. 1312. doi: 10.1016/j.ceramint.2017.08.084
    [46]
    X.R. Yang, C.W. Wang, P.F. Yan, et al., Pushing lithium cobalt oxides to 4.7V by lattice-matched interfacial engineering, Adv. Energy Mater., 12(2022), No. 23, art. No. 2200197. doi: 10.1002/aenm.202200197
    [47]
    H.J. Liang, Z.Y. Gu, X.X. Zhao, et al., Ether-based electrolyte chemistry towards high-voltage and long-life Na-ion full batteries, Angew. Chem. Int. Ed., 60(2021), No. 51, p. 26837. doi: 10.1002/anie.202112550
  • 加载中

Catalog

    通讯作者: 陈斌, bchen63@163.com
    • 1. 

      沈阳化工大学材料科学与工程学院 沈阳 110142

    1. 本站搜索
    2. 百度学术搜索
    3. 万方数据库搜索
    4. CNKI搜索

    Figures(6)

    Share Article

    Article Metrics

    Article Views(486) PDF Downloads(35) Cited by()
    Proportional views

    /

    DownLoad:  Full-Size Img  PowerPoint
    Return
    Return