Neighboring alkenyl group participated ether-based electrolyte for wide-temperature lithium metal batteries

Jimin Tang, Zhixuan Wei (), Junxiu Wu, Zhuangzhuang Cui, Ruiyuan Tian, Heng Jiang (), Fei Du () and Jun Lu ()
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Jimin Tang: Jilin University
Zhixuan Wei: Jilin University
Junxiu Wu: Zhejiang University
Zhuangzhuang Cui: University of Science and Technology of China
Ruiyuan Tian: Jilin University
Heng Jiang: Jilin University
Fei Du: Jilin University
Jun Lu: Zhejiang University

Nature Communications, 2025, vol. 16, issue 1, 1-12

Abstract: Abstract The extensive dendrite formation and unstable interfacial chemical environment pose significant obstacles to operating lithium metal batteries under extreme conditions. Here, we develop an allyl ether electrolyte operated across a wide-temperature range. Leveraging the neighboring group participation effect of alkenyl groups, the designed electrolyte possesses a quasi-weak solvation structure with low desolvation energy. Moreover, this effect facilitates the anion decomposition to form a dual-layer solid electrolyte interface, suppressing dendrite formation and surface parasitic reactions. Therefore, the single-salt, single-solvent electrolyte enables reversible lithium plating/stripping with high Coulombic efficiencies from −40 °C to 60 °C. The assembled 50 μm lithium | |3.5 mAh cm−2 sulfurized polyacrylonitrile full cells achieve capacity retention of 93.1% after 150 stable cycles (0.2 C) at 25 °C, where the positive electrode could retain 78% of its room temperature capacity at −40 °C. Moreover, the pouch cells demonstrate promising cycling stabilities, with a capacity retention of 94.8% (0.5 C), 92.4% (0.2 C), and 72.7% (0.1 C) after 100 cycles at 60 °C, 25 °C, and −40 °C, respectively. This terminal group modification strategy offers perspectives for wide-temperature electrolyte design, representing a crucial advancement in enhancing the performance of lithium metal batteries.

Date: 2025
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DOI: 10.1038/s41467-025-63262-z

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