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Designing safe and long-life lithium-ion batteries via a solvent-relay strategy

Nature Energy volume 10, pages 1450–1457 (2025)Cite this article

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Abstract

Ion association in highly concentrated electrolytes and localized highly concentrated electrolytes facilitates solid electrolyte interphase formation but compromises the thermal stability. Here we investigated the thermal behaviours of 20 electrolytes and uncovered that ion association lowers exothermic onset temperature by ~94 °C. To enhance the thermal stability without impairing solid electrolyte interphase formation, we developed a solvent-relay strategy that promotes ion association at ambient temperature while inducing dissociation at elevated temperatures. This approach enabled 4.5-V graphite-NCM811 pouch cells (1.1 Ah) to deliver 1,000 cycles under 0.45 C over 4,100 h with ~81.9% capacity retention and exceptional thermal safety, with a temperature rise lower than 3.5 °C during nail penetration, compared with 555.2 °C for commercial carbonate-based electrolytes. These findings elucidate the pivotal role of ion association in thermal runaway and offer a viable strategy to simultaneously achieve long cycle life, high-voltage operation and enhanced safety in ampere-hour-scale lithium-ion batteries.

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Fig. 1: Ion association promotes SEI formation while facilitating anion thermal decomposition.
Fig. 2: Correlation between ion association degree and onset temperatures.
Fig. 3: Anion decomposition pathways promoted by ion association.
Fig. 4: Solvent-relay strategy to prevent ion association at high temperatures.
Fig. 5: Electrochemical performance and abuse tests.

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Data availability

The datasets analysed and generated in this study are included in the paper and its Supplementary Information.

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Acknowledgements

The work described in this paper was supported by grants from the Research Grant Council (RGC) of the Hong Kong Special Administrative Region, China (project numbers RFS2223-4S03, R5019-22 and C1002-21G) and a grant from the Innovation and Technology Commission of the Hong Kong Special Administrative Region, China (project number ITS/219/21FP). Y.-C.L. acknowledges the support from Xplorer Prize by New Cornerstone Science Foundation.

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Authors and Affiliations

  1. Electrochemical Energy and Interfaces Laboratory, Department of Mechanical and Automation Engineering, The Chinese University of Hong Kong, Hong Kong SAR, China

    Yue Sun, Changjian Zuo, Huwei Wang, Liwei Jiang, Jing Xie & Yi-Chun Lu

  2. Institute of Materials Research and Engineering (IMRE), Agency for Science, Technology and Research (A*STAR), Singapore, Republic of Singapore

    Wanwan Wang

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Contributions

Y.S. and Y.-C.L. designed and conceived the experiments. C.Z. conducted pouch cell testing. W.W. conducted XPS tests. J.X. and L.J. conducted thermal analysis. H.W. conducted NMR, IR measurements and abuse tests. Y.S. and Y.-C.L. wrote the paper. Y.-C.L. supervised the project.

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Correspondence to Yi-Chun Lu.

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Nature Energy thanks Fei Wang, Guy Marlair and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary information

Supplementary Information (download PDF )

Supplementary Figs. 1–37, Notes 1–4 and Tables 1–7.

Supplementary Video 1 (download MP4 )

Videos showing nail penetration tests of 1.1 Ah graphite-NCM811 pouch cells using commercial electrolytes (1 M LiPF₆ in, 1:1 vol%) and GBF-D2 electrolyte.

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Sun, Y., Zuo, C., Wang, H. et al. Designing safe and long-life lithium-ion batteries via a solvent-relay strategy. Nat Energy 10, 1450–1457 (2025). https://doi.org/10.1038/s41560-025-01888-5

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