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Adaptive interphase enabled pressure-free all-solid-state lithium metal batteries

Nature Sustainability volume 8, pages 1360–1370 (2025)Cite this article

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Abstract

All-solid-state lithium metal (Li°) batteries (ASSLMBs) are a promising next-generation energy storage technology due to their use of non-flammable solid electrolytes for enhanced safety and the potential for higher energy density. However, void formation and evolution at the interface between anode and solid electrolyte remains a major challenge, leading to accelerated performance degradation. Departing from traditional interfacial design strategies, here we introduce dynamically adaptive interphases, formed by controllable migration of pre-installed anions in solid electrolytes, to operate ASSLMBs stably under low external pressure. The interphases adapt to the Li° anode volume changes, maintaining close physical contact between the Li° anode and ‘rigid’ solid electrolyte under low or zero external pressure. The dynamically adaptive interphase enables Li° full cells to deliver excellent rate performance and 90.7% of capacity retention after 2,400 cycles at a current density of 1.25 mA cm−2. Notably, pouch cells with zero external pressure are assembled with 74.4% of capacity retention after 300 cycles. The present work resolves the critical issue of the continuous solid–solid contact loss between Li° anodes and high-modulus solid electrolytes, advancing the practical deployment of ASSLMBs as high-energy, sustainable electrochemical storage systems.

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Fig. 1: First-principles calculations and experimental verification of anion migration in solid electrolytes.
Fig. 2: Electric field-driven migration of iodide ions to form iodide-rich DAIs.
Fig. 3: DAIs enabling excellent electrochemical cycling performance.
Fig. 4: Mechanistic understanding on DAI-stabilized ASSLMBs.

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Data availability

The data supporting the findings of this study are available within the article and its Supplementary Information. The relevant raw data are listed in Excel documents and provided as source or Supplementary Tables 1–3. Source data are provided with this paper.

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Acknowledgements

X.Y. acknowledges support from the National Key R&D Program of China (grant no. 2022YFB3807700), National Natural Science Foundation of China (grant no. 52372244) and Youth Innovation Promotion Association, Chinese Academy of Sciences (CAS) (grant no. Y2021080). H.Y. acknowledges support from the Youth Innovation Promotion Association, CAS (grant no. 2023009). L.B. acknowledges support from the National Natural Science Foundation of China (grant no. 22179144). R.X. acknowledges support from the Strategic Priority Research Program of CAS (grant no. XDB1040302). G.L. acknowledges support from the National Natural Science Foundation of China (grant no. 22309194).

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  1. These authors contributed equally: Guanjun Cen, Hailong Yu.

Authors and Affiliations

  1. Institute of Physics, Chinese Academy of Sciences, Beijing, China

    Guanjun Cen, Hailong Yu, Ruijuan Xiao, Jing Zhu, Xinxin Zhang & Xuejie Huang

  2. Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing, China

    Ruijuan Xiao, Xinxin Zhang, Xiayin Yao & Xuejie Huang

  3. Songshan Lake Materials Laboratory, Dongguan, China

    Liubin Ben & Xuejie Huang

  4. Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo, China

    Ronghan Qiao, Gaozhan Liu, Kemin Jiang & Xiayin Yao

  5. Key Laboratory of Material Chemistry for Energy Conversion and Storage (Ministry of Education), School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan, China

    Heng Zhang

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Contributions

X.H. conceived the original idea. X.H., H.Z. and X.Y. directed the work. H.Y. and G.C. designed the experiments. G.C., R.Q., J.Z., X.Z., G.L. and K.J. carried out the experiments and measurements. R.X. conducted the simulations. H.Y. and L.B. assisted with characterization. G.C., X.H., H.Z. and X.Y. wrote the initial draft, and all authors contributed to the writing of the final manuscript.

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Correspondence to Xiayin Yao, Heng Zhang or Xuejie Huang.

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Cen, G., Yu, H., Xiao, R. et al. Adaptive interphase enabled pressure-free all-solid-state lithium metal batteries. Nat Sustain 8, 1360–1370 (2025). https://doi.org/10.1038/s41893-025-01649-y

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