DOI: 10.1002/adma.202313135 ISSN: 0935-9648

A Fluoride‐Rich Solid‐Like Electrolyte Stabilizing Lithium Metal Batteries

Huashan Wang, Weiyuan Huang, Ruijun Rao, Jiacheng Zhu, Huige Chen, Haoyu Liu, Jiashuai Li, Qiufen Li, Mengxi Bai, Xiang Wang, Xuefeng Wang, Tongchao Liu, Khalil Amine, Ziqi Wang
  • Mechanical Engineering
  • Mechanics of Materials
  • General Materials Science


To address the problems associated with Li metal anodes, we present a fluoride‐rich solid‐like electrolyte (SLE) that combines the benefits of solid‐state and liquid electrolytes. Its unique triflate‐group‐enhanced frame channels facilitate the formation of a functional inorganic‐rich solid electrolyte interphase (SEI), which not only improves the reversibility and interfacial charge transfer of Li anodes but also ensures uniform and compact Li deposition. Furthermore, these triflate groups contribute to the decoupling of Li+ and provide hopping sites for rapid Li+ transport, enabling a high room‐temperature ionic conductivity of 1.1 mS cm−1 and a low activation energy of 0.17 eV, making it comparable to conventional liquid electrolytes. Consequently, Li symmetric cells using such SLE achieve extremely stable plating/stripping cycling over 3500 h at 0.5 mA cm−2 and support a high critical current up to 2.0 mA cm−2. The assembled Li||LiFePO4 solid‐like batteries exhibit exceptional cyclability for over one year and a half, even outperforming liquid cells. Additionally, high‐voltage cylindrical cells and high‐capacity pouch cells are demonstrated, corroborating much simpler processibility in battery assembly compared to all solid‐state batteries. These findings highlight the potential of the SLE approach in building a desirable SEI, offering practical solutions for the widespread adoption of rechargeable LMBs.

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