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Covariance of interphasic properties and fast chargeability of energy-dense lithium metal batteries

Nature Energy volume 10, pages 1132–1145 (2025)Cite this article

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Abstract

Lithium metal batteries can achieve high energy density, alleviating range anxiety for electric vehicles. However, the rational interphase design under fast charging conditions remains difficult. Here we explore a series of pyran-based electrolytes with various substitutional anions under a fast charging condition and observe weakly Li+-associating anions facilitating uniform lithium plating under a fast charging condition. We demonstrate lithium metal batteries achieving a 5–70% state of charge (SoC) within 12 min over 350 repeated cycles at a 4C (8.4 mA cm−2) charging rate, as well as high-energy designs delivering projected energy densities of 386 Wh kg−1 reaching a 10–80% SoC within 17 min over 180 cycles. We propose that the improved fast charging performance is in tandem with the ability of the weakly Li+ associating anions to suppress inorganic species clustering within the solid–electrolyte interphase and demonstrate the potential for electrolyte advancement based on the proposed mechanism.

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Fig. 1: Comparison of state-of-the-art Li metal and Li-ion batteries.
Fig. 2: Fast charging of the Li anode using state-of-the-art electrolytes.
Fig. 3: Fast charging of the Li anode using pyran-based electrolytes with various substitutional anions.
Fig. 4: Interphase on the Li metal anode in pyran-based electrolytes with various substitutional anions.
Fig. 5: Correlation analysis.
Fig. 6: MD simulations.
Fig. 7: Practical applicability of pyran-based electrolytes.

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The data supporting the findings of this study are included within the Article and its Supplementary Information and source data. Source data are provided with this paper.

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Acknowledgements

This work was supported by the LG Energy Solution-KAIST Frontier Research Laboratory (2022) and the National Foundation of Korea (NRF) grant funded by the Korea Ministry of Science and ICT (grant nos. 2022M3J1A1085404 and RS-2023-00261543, H.-T.K.). We thank G.-C. Chung, K. Nam Sohn and J. Young Kim for their support and comments on the research.

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Authors and Affiliations

  1. Department of Chemical and Biomolecular Engineering, KAIST, Daejeon, Republic of Korea

    Hyeokjin Kwon, Seongyeong Kim, Jonghyun Hyun, Yesom Kim, Il Ju Kim, Kyungjae Shin, Sejin Kim, Changhoon Park & Hee-Tak Kim

  2. Department of Mechanical Engineering, KAIST, Daejeon, Republic of Korea

    Ha Eun Lee & Seong Su Kim

  3. Battery R&D, LG Energy Solution, Daejeon, Republic of Korea

    Hongsin Kim & Dongseok Shin

  4. LG Energy Solution–KAIST Frontier Research Lab, KAIST, Daejeon, Republic of Korea

    Hee-Tak Kim

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  1. Hyeokjin Kwon
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Contributions

H. Kwon proposed the research, and H.-T.K. supervised the work. H. Kwon conducted the electrochemical tests, SEM and DFT simulations. H. Kwon and Seongyeong Kim performed and analysed the cryo-TEM, XPS and MD simulations. J.H., Y.K. and C.P. helped with the experiment design for the pouch cell test under pressurized conditions. H.E.L., S.S.K. and H. Kim contributed to the pouch cell testing fixture and pressure analysis. C.P., I.J.K., K.S. and Sejin Kim analysed the data. H. Kim and D.S. contributed to the battery design. H. Kwon and H.-T.K. co-wrote and revised the manuscript.

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Correspondence to Hee-Tak Kim.

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H.-T.K. and H. Kwon declare that this work has been filed for a KR Provisional Patent Application (no. 10-2024-0091552). The other authors declare no competing interests.

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Kwon, H., Kim, S., Hyun, J. et al. Covariance of interphasic properties and fast chargeability of energy-dense lithium metal batteries. Nat Energy 10, 1132–1145 (2025). https://doi.org/10.1038/s41560-025-01838-1

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