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High-energy, long-life Ni-rich cathode materials with columnar structures for all-solid-state batteries

Nature Energy volume 10, pages 479–489 (2025)Cite this article

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Abstract

All-solid-state batteries (ASSBs) comprising Ni-rich layered cathode active materials (CAMs) and sulfide solid electrolytes are promising candidates for next-generation batteries with high energy densities and safety. However, severe capacity fading occurs due to surface degradation at the CAM–electrolyte interface and severe lattice volume changes in the CAM, resulting in inner-particle isolation and detachment of the CAM from the electrolyte. Here we quantified the capacity fading factors of Ni-rich Li[NixCoyAl1−x−y]O2 composite ASSB cathodes as functions of Ni content. Surface degradation at the CAM–electrolyte interface was found to be the main cause of capacity fading in a CAM with 80% Ni content, whereas inner-particle isolation and detachment of the CAM from the electrolyte play a substantial role as the Ni content increases to 85% or more. On the basis of the comprehensive understanding of these mechanisms in ASSBs, high-performance Ni-rich CAMs with columnar structures were developed through surface and morphology modification.

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Fig. 1: Surface and morphology modification on NCA cathodes.
Fig. 2: Electrochemical performance of surface- and/or morphology-modified NCA cathodes.
Fig. 3: Degradation mechanism in ASSBs depending on Ni content in cathodes.
Fig. 4: Quantitative analysis of the three factors that affect capacity fading in ASSBs with Ni-rich cathodes.
Fig. 5: Crack formation behaviour in S-Ni90 and SM-Ni90 CAMs at the charged state.
Fig. 6: Quantitative analysis of the three factors that affect capacity fading in ASSBs depending on operating pressure.
Fig. 7: Long-term cycling test of dry-processed SM-Ni90 cathode with PTFE binder.
Fig. 8: Schematic illustration of strategies to overcome each factor of capacity fading in ASSBs.

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

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Acknowledgements

We thank W. Cho (Advanced Batteries Research Center, Korea Electronics Technology Institute) for pouch-type full-cell tests with a dry-processed electrode. This work was supported by the Human Resources Development Program (number 20214000000320; N.-Y.P., S.-M.P., Y.-K.S.) and ESS Big Data-Based O&M and Asset Management Technical Manpower Training (RS-2024-00398346; N.-Y.P., I.-S.L., Y.-K.S.) 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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  1. These authors contributed equally: Nam-Yung Park, Han-Uk Lee.

Authors and Affiliations

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

    Nam-Yung Park, Han-Uk Lee, Tae-Yeon Yu, In-Su Lee, Hun Kim, Sung-Min Park & Yang-Kook Sun

  2. Energy Storage Research Center, Korea Institute of Science and Technology, Seoul, South Korea

    Hun-Gi Jung

  3. Advanced Batteries Research Center, Korea Electronics Technology Institute, Seongnam, Republic of Korea

    Yun-Chae Jung

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

    Yang-Kook Sun

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Contributions

Y.-K.S. conceived and designed the research. H.-U.L., I.-S.L., S.-M.P., Y.-C.J. performed the experiments and characterization of materials. N.-Y.P., H.-U.L., T.-Y.Y, H.K. and H.-G.J. analysed the data. N.-Y.P., H.-U.L., T.-Y.Y, H.K. and Y.-K.S. contributed to the discussion of the results. N.-Y.P., T.-Y.Y. and H.K. wrote the original draft. N.-Y.P. and Y.-K.S. reviewed and edited the paper. All the authors commented on and revised the paper.

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Correspondence to Yang-Kook Sun.

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Park, NY., Lee, HU., Yu, TY. et al. High-energy, long-life Ni-rich cathode materials with columnar structures for all-solid-state batteries. Nat Energy 10, 479–489 (2025). https://doi.org/10.1038/s41560-025-01726-8

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