Skip to main content
Log in

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

  • Published:
International Journal of Minerals, Metallurgy and Materials Aims and scope Submit manuscript

Abstract

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.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Similar content being viewed by others

References

  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.

    Article  CAS  Google Scholar 

  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.

    Article  CAS  Google Scholar 

  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.

    Article  CAS  Google Scholar 

  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.

    Article  CAS  Google Scholar 

  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.

    Article  CAS  Google Scholar 

  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.

  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.

    Article  CAS  Google Scholar 

  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.

  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.

    Article  CAS  Google Scholar 

  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.

    Article  CAS  Google Scholar 

  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.

    Article  CAS  Google Scholar 

  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.

    Article  CAS  Google Scholar 

  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.

    Article  CAS  Google Scholar 

  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.

    Article  CAS  Google Scholar 

  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.

    Article  CAS  Google Scholar 

  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.

  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.

  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.

  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.

    Article  CAS  Google Scholar 

  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.

    Article  CAS  Google Scholar 

  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.

    Article  CAS  Google Scholar 

  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.

    Article  CAS  Google Scholar 

  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.

    Article  CAS  Google Scholar 

  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.

    Article  CAS  Google Scholar 

  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.

    Article  CAS  Google Scholar 

  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.

  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.

    Article  CAS  Google Scholar 

  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.

  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.

    Article  CAS  Google Scholar 

  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.

    Article  CAS  Google Scholar 

  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.

    Article  CAS  Google Scholar 

  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−xNarCoO2 by enlarging Li layer spacing, Electrochim. Acta, 273(2018), p. 145.

    Article  CAS  Google Scholar 

  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.

    Article  CAS  Google Scholar 

  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.

Download references

Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 51972030 and 51772030), the S&T Major Project of Inner Mongolia Autonomous Region in China (No. 2020ZD0018), the Beijing Outstanding Young Scientists Program (No. BJJWZYJH01201910007023), and the Guangdong Key Laboratory of Battery Safety (No. 019B121203008).

Author information

Authors and Affiliations

Authors

Corresponding authors

Correspondence to Renjie Chen or Li Li.

Additional information

Conflict of Interest

The authors declare no competing interests.

Supplementary Information

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Lin, J., Wu, J., Fan, E. et al. Environmental and economic assessment of structural repair technologies for spent lithium-ion battery cathode materials. Int J Miner Metall Mater 29, 942–952 (2022). https://doi.org/10.1007/s12613-022-2430-7

Download citation

  • Received:

  • Revised:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s12613-022-2430-7

Keywords

Navigation