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<p>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<sup>+</sup>-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 (-CF<sub>3</sub>) 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 -CF<sub>3</sub>, we find that its lithiophobic nature against Li<sup>+</sup> 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<sup>+</sup> 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 &gt;400 cycles under fast-charging condition, and &gt;100 cycles in 14-Ah-level industrial pouch cell with a high energy density over 510 Wh kg<sup>−1</sup> at cell-level.</p>

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

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年5月21日

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  • 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,
  • Yonghong Deng

摘要

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.