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

Miao Du, Hongyan Lü, Kaidi Du, Shuohang Zheng, Xiaotong Wang, Xiaotong Deng, Ronghua Zeng, Xinglong Wu

International Journal of Minerals, Metallurgy, and Materials ›› 2024, Vol. 31 ›› Issue (7) : 1745-1751. DOI: 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 information +
History +

Abstract

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 Li+/PF6 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.

Keywords

recycle / lithium cobalt oxide / lithium cobalt phosphate / graphite / dual-ion batteries / spent lithium-ion batteries

Cite this article

Download citation ▾
Miao Du, Hongyan Lü, Kaidi Du, Shuohang Zheng, Xiaotong Wang, Xiaotong Deng, Ronghua Zeng, Xinglong Wu. Upcycling the spent graphite/LiCoO2 batteries for high-voltage graphite/LiCoPO4-co-workable dual-ion batteries. International Journal of Minerals, Metallurgy, and Materials, 2024, 31(7): 1745‒1751 https://doi.org/10.1007/s12613-023-2807-2

References

[[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.
[[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.
[[3]]
Lu QP, Du ZH, Wang J, et al.. Editorial for special issue on renewable energy conversion, utilization and storage. Int. J. Miner. Metall. Mater., 2023, 30(10): 1855,
CrossRef Google scholar
[[4]]
Yu ZZ, Zhao GQ, Ji FL, et al.. Collaboratively enhancing electrochemical properties of LiNi0.83Co0.11Mn0.06O2 through doping and coating of quadrivalent elements. Rare Met., 2023, 42(12): 4103,
CrossRef Google scholar
[[5]]
Zhang R, Wang CY, Zou PC, et al.. Compositionally complex doping for zero-strain zero-cobalt layered cathodes. Nature, 2022, 610(7930): 67,
CrossRef Pubmed Google scholar
[[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.
[[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.
[[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.
[[9]]
Zhang KY, Xu YZ, Lin YC, et al.. Enriching redox active sites by interconnected nanowalls-like nickel cobalt phosphosulfide nanosheets for high performance supercapacitors. Chin. Chem. Lett., 2021, 32(11): 3553,
CrossRef Google scholar
[[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.
[[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.
[[12]]
Xiang M, Fan WX, Lin W, et al.. Triple kill: Fabrication of composites coming from waste face masks, polystyrene microplastics, graphene, and their electromagnetic interference shielding behaviors. Carbon Neutralization, 2023, 2(5): 616,
CrossRef Google scholar
[[13]]
Du KD, Ang EH, Wu XL, Liu YC. Progresses in sustainable recycling technology of spent lithium-ion batteries. Energy Environ. Mater., 2022, 5(4): 1012,
CrossRef Google scholar
[[14]]
Wang J, Yuan YF, Rao XH, et al.. Realizing high-performance Na3V2(PO4)2O2F cathode for sodium-ion batteries via Nb-doping. Int. J. Miner. Metall. Mater., 2023, 30(10): 1859,
CrossRef Google scholar
[[15]]
Yang YN, Yang YJ, He CL, 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., 2023, 30(5): 897,
CrossRef Google scholar
[[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]]
Baum ZJ, Bird RE, Yu X, Ma J. Lithium-ion battery recycling—Overview of techniques and trends. ACS Energy Lett., 2022, 7(2): 712,
CrossRef Google scholar
[[18]]
Costa CM, Barbosa JC, Gonçalves R, Castro H, del Campo FJ, Lanceros-Méndez S. Recycling and environmental issues of lithium-ion batteries: Advances, challenges and opportunities. Energy Storage Mater., 2021, 37: 433,
CrossRef Google scholar
[[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.
[[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.
[[21]]
Wang XT, Gu ZY, Ang EH, Zhao XX, Wu XL, Liu YC. Prospects for managing end-of-life lithium-ion batteries: Present and future. Interdiscip. Mater., 2022, 1(3): 417,
CrossRef Google scholar
[[22]]
Zhong T, Zhang HY, Song MC, et al.. FeCoNiCrMo high entropy alloy nanosheets catalyzed magnesium hydride for solid-state hydrogen storage. Int. J. Miner. Metall. Mater., 2023, 30(11): 2270,
CrossRef Google scholar
[[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.
[[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.
[[26]]
Dang H, Chang ZD, Zhou HL, Ma SH, Li M, Xiang JL. Extraction of lithium from the simulated pyrometallurgical slag of spent lithium-ion batteries by binary eutectic molten carbonates. Int. J. Miner. Metall. Mater., 2022, 29(9): 1715,
CrossRef Google scholar
[[27]]
Du KD, Meng YF, Zhao XX, et al.. A unique co-recovery strategy of cathode and anode from spent LiFePO4 battery. Sci. China Mater., 2022, 65(3): 637,
CrossRef Google scholar
[[28]]
Lin J, Wu JW, Fan ES, et al.. Environmental and economic assessment of structural repair technologies for spent lithiumion battery cathode materials. Int. J. Miner. Metall. Mater., 2022, 29(5): 942,
CrossRef Google scholar
[[29]]
T. Wang, H.M. Luo, Y.C. Bai, J.L. Li, I. Belharouak, and S. Dai, Direct recycling of spent NCM cathodes through iono-thermal lithiation, Adv. Energy Mater., 10(2020), No. 30, art. No. 2001204.
[[30]]
Xu B, Dong P, Duan JG, Wang D, Huang XS, Zhang YJ. Regenerating the used LiFePO4 to high performance cathode via mechanochemical activation assisted V5+ doping. Ceram. Int., 2019, 45(9): 11792,
CrossRef Google scholar
[[31]]
Meng XQ, Cao HB, Hao J, Ning PG, Xu GJ, Sun Z. 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., 2018, 6(5): 5797,
CrossRef Google scholar
[[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.
[[33]]
Gu ZY, Guo JZ, Zhao XX, et al.. High-ionicity fluorophos-phate lattice via aliovalent substitution as advanced cathode materials in sodium-ion batteries. InfoMat, 2021, 3(6): 694,
CrossRef Google scholar
[[34]]
Guo MC, Tang W, Hong Y, et al.. Self-carbonization of soluble organic cathodes enables stable Na-ion batteries. Sci. China Mater., 2023, 66(7): 2621,
CrossRef Google scholar
[[35]]
Yang Y, Guo JZ, Gu ZY, 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., 2019, 7(14): 12014
[[36]]
Du M, Du KD, Guo JZ, et al.. Direct reuse of oxide scrap from retired lithium-ion batteries: Advanced cathode materials for sodium-ion batteries. Rare Met., 2023, 42(5): 1603,
CrossRef Google scholar
[[37]]
Yang JL, Zhao XX, Li WH, et al.. Advanced cathode for dual-ion batteries: Waste-to-wealth reuse of spent graphite from lithium-ion batteries. eScience, 2022, 2(1): 95,
CrossRef Google scholar
[[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.
[[39]]
Meng YF, Liang HJ, Zhao CD, 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., 2022, 64: 166,
CrossRef Google scholar
[[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.
[[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.
[[42]]
J.Z. Guo, H.X. Zhang, Z.Y. Gu, et al., Heterogeneous NAS-ICON-type composite as low-cost, high-performance cathode for sodium-ion batteries, Adv. Funct. Mater., 32(2022), No. 52, art. No. 2209482.
[[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.
[[44]]
Priyadharsini N, Shanmugapriya S, Kasturi PR, Surendran S, Selvan RK. Morphology-dependent electrochemical properties of sol-gel synthesized LiCoPO4 for aqueous hybrid capacitors. Electrochim. Acta, 2018, 289: 516,
CrossRef Google scholar
[[45]]
Wang Y, Qiu JY, Yu ZB, et al.. AlF3-modified LiCoPO4 for an advanced cathode towards high energy lithium-ion battery. Ceram. Int., 2018, 44(2): 1312,
CrossRef Google scholar
[[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.
[[47]]
Liang HJ, Gu ZY, Zhao XX, et al.. Ether-based electrolyte chemistry towards high-voltage and long-life Na-ion full batteries. Angew. Chem. Int. Ed., 2021, 60(51): 26837,
CrossRef Google scholar

Accesses

Citations

Detail

Sections
Recommended

/