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Near-surface reconstruction in Ni-rich layered cathodes for high-performance lithium-ion batteries

Nature Energy volume 9, pages 47–56 (2024)Cite this article

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Abstract

The instability of the Ni-rich layered cathode materials in lithium-ion batteries is attributed to their labile surface reactivity. This reactivity induces the formation of residual lithium impurities on the cathode surface and severe side reactions with the electrolyte. Here we propose a washing process using Co-dissolved water for simultaneously removing residual lithium and forming a protective coating on Ni-rich layered cathodes. The washing induces the reconstruction of the near-surface structure through reactions with the residual lithium compounds, thereby preventing direct contact between the electrolyte and the Ni-rich surface. An additional fluorine coating on the washed cathode impedes the decomposition of salts, preventing the by-products from triggering autocatalytic side reactions at the electrolyte–cathode interface and thereby suppressing gas generation during cycling. The combination of these near-surface reconstructions synergistically extends the cycle lives of Ni-rich cathodes and satisfies the requirements concerning energy density, durability and safety for next-generation batteries in practical applications.

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Fig. 1: Formation of Co-rich layer on the cathode surface.
Fig. 2: Characterizations of the reconstructed near-surface properties.
Fig. 3: Comparison of electrochemical performances depending on surface modifications.
Fig. 4: Post-mortem analyses of the cycled cathode.
Fig. 5: Investigation of the preformed LiF effect on the cathode surface through XPS depth analysis.
Fig. 6: Long-term cycling performance and swelling during cycling.

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All data generated or analysed during this study are included in the published article and its Supplementary Information. Source data are provided with this paper.

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Acknowledgements

This work and all authors were supported by the Human Resources Development Program (number 20214000000320) of the Korea Institute of Energy Technology Evaluation and Planning (KETEP), funded by the Ministry of Trade, Industry and Energy of the Korean government.

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Authors and Affiliations

  1. Department of Energy Engineering, Hanyang University, Seoul, South Korea

    Hoon-Hee Ryu, Hyung-Woo Lim, Sin Gyu Lee & Yang-Kook Sun

  2. Department of Battery Engineering, Hanyang University, Seoul, South Korea

    Yang-Kook Sun

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Contributions

H.-H.R. and Y.-K.S. conceived and designed the research. H.-H.R., H.-W.L. and S.G.L. performed the experiments and characterization of materials. H.-H.R. and H.-W.L. analysed the data. H.-H.R., H.-W.L., S.G.L. and Y.-K.S. contributed to the discussion of the results. H.-H.R. wrote the original draft, and Y.-K.S. reviewed and edited the manuscript. All the authors commented on and revised the manuscript.

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Correspondence to Yang-Kook Sun.

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Competing interests

The authors have filed provisional patent applications: Y.-K.S. and H.-H.R. are inventors of a patent application (Korean patent application 10-2023-0128916) on the experimental methods for washing and coating herein. The other authors declare no competing interests.

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Nature Energy thanks Xifei Li, Philipp Kurzhals and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Ryu, HH., Lim, HW., Lee, S.G. et al. Near-surface reconstruction in Ni-rich layered cathodes for high-performance lithium-ion batteries. Nat Energy 9, 47–56 (2024). https://doi.org/10.1038/s41560-023-01403-8

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