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Long-cycling lithium-metal batteries via an integrated solid–electrolyte interphase promoted by a progressive dual-passivation coating

Nature Energy volume 10, pages 941–950 (2025)Cite this article

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Abstract

Stabilizing lithium (Li) metal anodes has long been hindered by the challenge of forming a stable solid–electrolyte interphase, stemming from the inherently high reactivity of Li metal with liquid electrolytes. Here we developed a progressive dual-passivation polymer coating strategy to stabilize Li-metal anodes, achieving exceptional cycle life of Li-metal batteries in carbonate electrolyte. Unlike current approaches, the synthesized copolymer coating passivates the Li-metal anode while also tailoring the Li-ion solvation structure by facilitating selective anion decoordination in a binary salt carbonate electrolyte. This process leads to the formation of an integrated solid–electrolyte interphase, featuring a chemical passivation outer layer predominant in LiF generated by the polymer coating and an anion-derived Li2O-prevalent inner layer from the electrolyte decomposition. Consequently, this coating strategy remarkably enhances the stability of Li-metal anodes, enabling double-layer Li||NMC811 pouch cells to maintain 80% of their initial capacity up to 611 cycles under a low electrolyte/capacity (E/C) ratio of 2.0 g Ah−1.

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Fig. 1: Schematic illustrations of the progressive dual-passivation coating strategy to form an integrated SEI for stabilizing Li-metal anode in a binary salt carbonate electrolyte.
Fig. 2: The chemical structure and characterization of polymers PFSPA and PFSPO.
Fig. 3: The XPS and AFM characterizations of the SEI layers.
Fig. 4: Studies on Li deposition morphology and the chemistry of the formed SEI.
Fig. 5: Electrochemical performance evaluation of the Li||NMC811 full cells with and without coatings.

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All data supporting the conclusions of this study are provided within the main article and its Supplementary Information files.

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Acknowledgements

This work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the US Department of Energy, through the Advanced Battery Materials Research Program (Battery500 Consortium) and Battelle-Pacific Northwest National Laboratory Subcontract Award (614551, 790825, D.W.). Y.-S.L., J.L. and S.H.K. acknowledge support from the National Science Foundation (grant number CMMI-2038494, S.H.K.).

Author information

Authors and Affiliations

  1. Department of Mechanical Engineering, The Pennsylvania State University, University Park, PA, USA

    Guo-Xing Li & Donghai Wang

  2. Department of Mechanical Engineering, Southern Methodist University, Dallas, TX, USA

    Rong Kou & Donghai Wang

  3. Department of Materials Science and Engineering, The Pennsylvania State University, University Park, PA, USA

    Au Nguyen

  4. Materials Research Institute, The Pennsylvania State University, University Park, PA, USA

    Ke Wang

  5. Department of Chemical Engineering and Materials Research Institute, The Pennsylvania State University, University Park, PA, USA

    Yu-Sheng Li, Jongcheol Lee & Seong H. Kim

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  1. Guo-Xing Li
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Contributions

G.-X.L. and D.W. developed and designed the concept for this study. G.-X.L. and R.K. performed the electrochemical evaluation, 1H and 19F NMR analysis. A.N. performed and analysed the XPS characterization. K.W. performed and analysed the cryo-TEM characterization. Under the supervision of S.H.K., Y.-S.L. and J.L. performed the AFM characterization and wrote the corresponding experimental section. G.-X.L. and D.W. wrote and revised the paper.

Corresponding author

Correspondence to Donghai Wang.

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Nature Energy thanks Jong-Won Lee and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Information

Supplementary Figs. 1–41, Table 1 and Discussion.

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Li, GX., Kou, R., Nguyen, A. et al. Long-cycling lithium-metal batteries via an integrated solid–electrolyte interphase promoted by a progressive dual-passivation coating. Nat Energy 10, 941–950 (2025). https://doi.org/10.1038/s41560-025-01803-y

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