Abstract
In high-voltage lithium-metal battery systems, electrolyte characteristics are crucial for achieving the optimal balance between non-flammability and battery performance. Herein, an electrolyte system based on triethyl phosphate solvent with lithium oxide difluoroborate, lithium tetrafluoroborate and lithium nitrate as solutes is proposed. TEP, as the sole solvent, ensures the inherent non-flammability of the electrolyte, while the solutes LiODFB, LiBF4 and LiNO3, benefit from the different binding energies of the three anions and lithium ions, to optimize the structure of the solvation shell and direction of anion movement, thereby forming a favorable interfacial phase. Consequently, solid electrolyte interphase enriched with B-O and Li3N in the inner layer and LiF in the outer layer is formed, which improves the stability and reversibility of the lithium metal negative electrode. The Li | |NCM811 cell with the as-prepared electrolyte can be stably cycled for 600 cycles at a high cut-off voltage of 4.5 V with a capacity retention of 90.19%. Even at 60 °C for 600 cycles, the capacity retention rate remains at 81.18%. This work demonstrates an effective strategy for the design of high-voltage non-flammable LMBs.
Data availability
All data that support the findings of this study are presented in the manuscript and Supplementary Information, or are available from the corresponding author upon request. Source data are provided with this paper.
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Acknowledgements
This work was supported by the National Natural Science Foundation of China (92372207 and 22075174), the Science and Technology Commission of Shanghai Municipality (20520740900 and 19DZ2271100), the China Postdoctoral Science Foundation (2024T170794 and 2024M762822), the Zhejiang Province Postdoctoral Scientific Research Project (ZJ2024049), and the International Joint Laboratory on Resource Chemistry. We thank the Quzhou Institute of Power Battery and Grid Energy Storage for providing the pouch cells.
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S.X. conceived the idea, performed the experiment, and wrote the manuscript. Q.G. and S.G. performed molecular dynamics simulations. L.Z., R.G., and X.G. contributed to the results discussion and data analysis. J.X., S.Z., Q.X., P.S., X.Z., Y.M., and J.L. supervised this work, discussed the results, and revised this manuscript.
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Xu, S., Zheng, L., Guo, X. et al. Customized composition of lithium metal solid-electrolyte interphase by electric field modulation of anion motion direction. Nat Commun (2026). https://doi.org/10.1038/s41467-026-68498-x
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DOI: https://doi.org/10.1038/s41467-026-68498-x
