Li2ZrF6-based electrolytes for durable lithium metal batteries

Qingshuai Xu, Tan Li, Zhijin Ju, Guangxu Chen, Daiqi Ye, Geoffrey I. N. Waterhouse, Yingying Lu, Xuejun Lai, Guangmin Zhou, Lin Guo (), Keyou Yan (), Xinyong Tao (), Hong Li () and Yongcai Qiu
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Qingshuai Xu: South China University of Technology
Tan Li: South China University of Technology
Zhijin Ju: Wenzhou University
Guangxu Chen: South China University of Technology
Daiqi Ye: South China University of Technology
Geoffrey I. N. Waterhouse: The University of Auckland
Yingying Lu: Zhejiang University
Xuejun Lai: South China University of Technology
Guangmin Zhou: Tsinghua University
Lin Guo: Beihang University
Keyou Yan: South China University of Technology
Xinyong Tao: Zhejiang University of Technology
Hong Li: Chinese Academy of Sciences
Yongcai Qiu: South China University of Technology

Nature, 2025, vol. 637, issue 8045, 339-346

Abstract: Abstract Lithium (Li) metal batteries (LMBs) are promising for high-energy-density rechargeable batteries1–3. However, Li dendrites formed by the reaction between highly active Li and non-aqueous electrolytes lead to safety concerns and rapid capacity decay4–7. Developing a reliable solid–electrolyte interphase is critical for realizing high-rate and long-life LMBs, but remains technically challenging4,8. Here we demonstrate that adding excess m-Li2ZrF6 (monoclinic) nanoparticles to a commercial LiPF6-containing carbonate electrolyte of LMBs facilitates the release of abundant ZrF62– ions into the electrolyte driven by the applied voltage, converting to t-Li2ZrF6 (trigonal) and creating a stable solid–electrolyte interphase in situ with high Li-ion conductivity. Computational and cryogenic transmission electron microscopy studies revealed that the in situ formation of the t-Li2ZrF6-rich solid–electrolyte interphase markedly enhanced Li-ion transfer and suppressed the growth of Li dendrites. As a result, LMBs assembled with LiFePO4 cathodes (areal loading, 1.8/2.2 mAh cm−2), three-dimensional Li–carbon anodes (50-µm-thick Li) and Li2ZrF6-based electrolyte displayed greatly improved cycling stability with high capacity retention (>80.0%) after 3,000 cycles (1C/2C rate). This achievement represents leading performance and, thus, delivers a reliable Li2ZrF6-based electrolyte for durable LMBs under practical high-rate conditions.

Date: 2025
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DOI: 10.1038/s41586-024-08294-z

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