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A universal protocol for ultrafast direct regeneration and upcycling of spent lithium-ion battery cathode materials

Nature Protocols (2025)Cite this article

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Abstract

The rapid acceleration of global electrification has increased demand for sustainable energy storage, making lithium-ion batteries (LIBs) essential for various applications. However, their limited lifespan presents challenges related to resource waste and environmental risks. Unlike traditional metallurgical methods, which extract key metals from spent cathodes, the direct recycling process repairs damaged materials, maximizing their residual value through effective treatments. Despite widespread interest, systematic protocols to guide interdisciplinary researchers in direct recycling studies remain scarce. Using spent LiMn2O4 as an example, this protocol outlines a general approach for direct recycling and upcycling of spent LIBs. Initially, the failure condition of the spent cathode is evaluated using X-ray diffraction and inductively coupled plasma analysis to determine appropriate recycling parameters. The resulting recycled products include regenerated LiMn2O4 and upcycled next-generation cathode materials, such as high-voltage LiNi0.5Mn1.5O4 and Co-free, Li-rich Li1.2Ni0.2Mn0.6O2. Subsequently, electron microscopy, spectroscopic techniques and electrochemical performance tests evaluate recycling effectiveness. This protocol incorporates two representative recycling methods to provide readers with a detailed procedural guide. Solid-phase regeneration forms the basis of most direct recycling technologies; thus, it requires minimal adjustments for broad applicability. Joule heating, a more emerging recycling technology, leverages rapid nonequilibrium reactions, substantially reducing processing time and introducing beneficial structural defects and elemental gradient distributions within the material. Compared to metallurgical methods, solid-phase and Joule heating-based protocols reduce recycling time to ~32 h and 5 h, respectively. Overall, this protocol provides a reliable guide for researchers, promoting sustainable LIB recycling and advancing clean energy research.

Key points

  • This protocol introduces two representative techniques to help readers easily adapt and optimize the methods for implementing a direct recycling process.

  • The success of direct recycling hinges on thorough pretreatment and addressing the challenges posed by the failure behavior of spent materials, including lithium replenishment and phase structure recovery.

  • The core of direct upcycling lies in constructing a viable direct phase evolution path between the target and initial materials.

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Fig. 1: A comparison of spent LIB recycling technologies at different stages of development.
Fig. 2: The overall experimental design of this protocol.
Fig. 3: Failure analysis of spent cathode materials.
Fig. 4: Structural characterization of regenerated LiMn2O4 cathode materials.
Fig. 5: Electrochemical performance of regenerated LiMn2O4 cathode materials.
Fig. 6: Structural characterization of upcycled high-voltage cathode material LiNi0.5Mn1.5O4.
Fig. 7: Electrochemical performance of upcycled high-voltage cathode material LiNi0.5Mn1.5O4.
Fig. 8: Structural characterization of upcycled Li-rich Mn-based cathode material Li1.2Ni0.2Mn0.6O2.
Fig. 9: Electrochemical performance of upcycled Li-rich Mn-based cathode material Li1.2Ni0.2Mn0.6O2.

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Data availability

All of the data supporting this research are available in the main text and the Supplementary Information, and original data can be obtained from the corresponding authors upon reasonable request. Source data are provided with this paper. Other data supporting the findings of this study were previously published28,35,46,48. Source data are provided with this paper.

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Acknowledgements

G.Z. was supported by the Guangdong Innovative and Entrepreneurial Research Team Program (grant no. 2021ZT09L197), Shenzhen Science and Technology Program (grant no. KQTD20210811090112002), the Interdisciplinary Research and Innovation Fund of Tsinghua Shenzhen International Graduate School and the Tsinghua Shenzhen International Graduate School-Shenzhen Pengrui Young Faculty Program of Shenzhen Pengrui Foundation (grant no. SZPR2023007). H.J. was supported by the National Natural Science Foundation of China (grant no. 524B2023). J.W. was supported by the Startup Fund for Young Faculty at Shanghai Jaio Tong University (grant no. 23×010502206) and the National Natural Science Youth Fund (grant no. 52302285).

Author information

Author notes

  1. These authors contributed equally: Haocheng Ji, Junxiong Wang.

Authors and Affiliations

  1. Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, China

    Haocheng Ji, Junxiong Wang, Hao Zhang, Guanjun Ji & Guangmin Zhou

  2. Frontiers Science Center for Transformative Molecules, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, China

    Junxiong Wang & Guanjun Ji

  3. Department of Electronic and Computer Engineering, The Hong Kong University of Science and Technology, Kowloon, Hong Kong SAR, China

    Xiao Qiu

  4. School of Advanced Materials, Peking University Shenzhen Graduate School, Shenzhen, China

    Hengyu Ren & Haoyu Xue

  5. Faculty of Materials Science and Energy Engineering and Institute of Technology for Carbon Neutrality, Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen, China

    Hui-Ming Cheng

  6. Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang, China

    Hui-Ming Cheng

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Contributions

H.J., J.W., G.Z. and H.-M.C. conceived the idea and provided design guidelines. H.J. and J.W. performed the relevant experiments and data analysis with the help of X.Q., H.R., H.X., H.Z. and G.J. All authors discussed and contributed to the results. H.J. wrote the manuscript with comments and revisions from all the authors.

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Correspondence to Hui-Ming Cheng or Guangmin Zhou.

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Nature Protocols thanks Hao Luo and Min-Sik Park for their contribution to the peer review of this work.

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Key references

Wang, J. et al. Nat. Sustain. 7, 1283–1293 (2024): https://doi.org/10.1038/s41893-024-01412-9

Wang, J. et al. Nat. Sustain. 6, 797–805 (2023): https://doi.org/10.1038/s41893-023-01094-9

Ma, J. et al. Nat. Commun. 15, 1046 (2024): https://doi.org/10.1038/s41467-024-45091-8

Choi, C. H. et al. Nat. Chem. 16, 1831–1837 (2024): https://doi.org/10.1038/s41557-024-01598-7

Wang, C. et al. Science 369, 521–526 (2020): https://doi.org/10.1126/science.aaz7681

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Ji, H., Wang, J., Qiu, X. et al. A universal protocol for ultrafast direct regeneration and upcycling of spent lithium-ion battery cathode materials. Nat Protoc (2025). https://doi.org/10.1038/s41596-025-01234-9

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