High-energy and fast-charging lithium metal batteries enabled by tuning Li+-solvation via electron-withdrawing and lithiophobicity functionality

Guangzhao Zhang, Tong Zhang, Zhen Zhang, Ruilin He, Qingrong Wang, Shang-Sen Chi, Yanming Cui (), Meng Danny Gu, Zhongbo Liu, Jian Chang, Chaoyang Wang (), Kang Xu () and Yonghong Deng ()
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Guangzhao Zhang: Southern University of Science and Technology
Tong Zhang: Southern University of Science and Technology
Zhen Zhang: Southern University of Science and Technology
Ruilin He: Southern University of Science and Technology
Qingrong Wang: Southern University of Science and Technology
Shang-Sen Chi: Southern University of Science and Technology
Yanming Cui: Ltd.
Meng Danny Gu: Eastern Institute of Technology
Zhongbo Liu: Shenzhen CAPCHEM Technology Co. Ltd
Jian Chang: Great Bay University
Chaoyang Wang: South China University of Technology
Kang Xu: SolidEnergy Systems LLC
Yonghong Deng: Southern University of Science and Technology

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

Abstract: Abstract The solvent fluorination almost always improves electrochemical stability of electrolytes against both lithium anodes and high-voltage cathodes in lithium metal batteries. However, how exactly fluorination affects Li+-solvation and interphasial chemistries remains unclear, hindering rational design of electrolytes and interphases with both wide electrochemical stability window and fast ion transport kinetics that are required for energy-dense and fast-charging LMBs. Here we introduce the trifluoromethylation (-CF3) at one end of 1,2-dimethoxyethane and generate 1,1,1-trifluoro-2-(2-methoxyethoxy) ethane, which as a single solvent of electrolyte simultaneously meets energy-dense and fast-charging requirements when dissolving 2 M lithium bis(fluorosulfonyl)imide. Beside the electron-withdrawing effect of -CF3, we find that its lithiophobic nature against Li+ significantly alters the solvation structures, which favors the formation of anion-dominated clusters that lead to superior interphasial chemistries in layered structure and fast Li+ transport kinetics. In such electrolyte, lithium metal batteries constructed with 50-μm-thin Li||high-loading-NMC811 in both coin and pouch cell configurations achieve >400 cycles under fast-charging condition, and >100 cycles in 14-Ah-level industrial pouch cell with a high energy density over 510 Wh kg−1 at cell-level.

Date: 2025
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DOI: 10.1038/s41467-025-59967-w

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