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Sustainable regeneration of spent cathodes for lithium-ion and post-lithium-ion batteries

Abstract

The accelerating adoption of electric vehicles supports the transition to a more sustainable transport sector. However, the retiring of many electric vehicles over the next decade poses a sustainability challenge, particularly due to the lack of recycling of end-of-life batteries. Here we show regeneration routes that could valorize spent cathodes for a second life in both lithium-ion batteries (LIBs) and post-LIBs. Our regeneration starts with a leaching process involving acetic acid that could selectively dissolve high-value elements in cathodes including lithium, cobalt, nickel and manganese. Depending on the added chelating agents, further co-precipitation reactions in the leachate form precursors of different cathode materials. The regenerated lithium layered oxide cathodes deliver a reversible area capacity of up to 2.73 mAh cm−2 with excellent structural stability for LIBs, whereas the obtained Prussian blue analogues show 83.7% retention after 2,000 cycles for sodium-ion batteries (SIBs). Life-cycle and techno-economic assessments suggest that the current regeneration can reduce manufacturing costs for LIBs and SIBs by US$21.65 kWh−1 and US$41.67 kWh−1, respectively, with lower impacts on human health, environment and natural resources. This work paves the way for the transition to more sustainable storage technologies.

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Fig. 1: Extraction of high-value elements.
Fig. 2: Regenerated cathode materials for LIBs.
Fig. 3: Regenerated cathode materials for post-LIBs.
Fig. 4: Evaluation of cathode regeneration technologies.

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Data availability

The data supporting the research in this paper are available within the article and its Supplementary Information or from the corresponding authors upon reasonable request. Source data are provided with this paper.

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Acknowledgements

Z.C. acknowledges the support from the Power Battery and Systems Research Center from State Key Laboratory of Catalysis, Strategic Priority Research Program of Chinese Academy of Sciences (XDB0600104), Dalian Revitalization Talents Program (2022RG01), Liaoning Binhai Laboratory (LBLB202304), Vacuum Interconnected Nanotech Workstation (Nano-X, Suzhou Institute of Nano-Tech and Nano-Bionics), the Natural Sciences and Engineering Research Council of Canada (NSERC), the University of Waterloo and the Waterloo Institute for Nanotechnology. Allocation of beamtime at HXMA, SXRMB and VESPERS, CLS, Saskatoon, Canada, is gratefully acknowledged. We also thank Shiyanjia Lab (www.shiyanjia.com) for the LCA.

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Authors

Contributions

T.Y., Y.Z. and Z.C. designed the research. T.Y. and Z.C. completed most of the experiments and drafted the paper. D.L., Q.M. and R.G. assisted in the design of some advanced characterization methods and provided extensive suggestions for the paper. Z.C., X.Z., S.G. and T.O. supervized the project and assembled the pouch cells. Z.C., D.L. and H.W.P. made significant contributions to the analysis and editing of the paper. All authors discussed and contributed to the results.

Corresponding authors

Correspondence to Yongguang Zhang or Zhongwei Chen.

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Nature Sustainability thanks the anonymous reviewers for their contribution to the peer review of this work.

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Supplementary information

Supplementary Information

Supplementary Figs. 1–54 and Tables 1–46.

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Source data

Source Data Fig. 1

ICP results.

Source Data Fig. 2

Electrochemical performance of LIBs.

Source Data Fig. 3

Electrochemical performance of SIBs.

Source Data Fig. 4

Techno-economic analysis and LCA results.

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Yang, T., Luo, D., Zhang, X. et al. Sustainable regeneration of spent cathodes for lithium-ion and post-lithium-ion batteries. Nat Sustain 7, 776–785 (2024). https://doi.org/10.1038/s41893-024-01351-5

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