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<p>Enhancing cycling reversibility in high-energy-density lithium metal batteries necessitates precise management of electrolyte-derived electrochemical reactions at electrodes and interphases, yet recently developed localized high-concentration electrolytes suffer from limited tunability of these reactions for the non-solvation-participating nature of oxygen-proximal fluorinated diluents. Here we address this issue by synthesizing an oxygen-distal fluorinated di-2,2,3,3-tetrafluoropropoxyethane diluent whose molecular skeleton is strategically edited to position fluorine atoms distal to oxygen centers that attenuate electron-withdrawing effects at Li<sup>+</sup>-coordination sites, enabling: enhanced diluent/anion participation and reduced volatile solvents in solvation shells; atypical H-F bonding between diluent and solvent toward enhanced oxidation resistance; and promotion of diluent and salt-derived highly stable inorganic-rich interphase formation. This electrolyte achieves 99.8% Li plating/stripping Coulombic efficiency, 450 stable cycles in 4.5 V high-voltage Li || LiNi<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub> cells, and 5.9-Ah, 504.6 Wh kg<sup>–1</sup> (based on mass of all components including packaging) pouch cells that exhibits 0.053% per-cycle capacity decay. This work introduces oxygen-distal fluorination as a potential molecular skeleton editing strategy for stable energy-dense lithium metal batteries.</p>

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Skeletal editing of ether-based electrolyte diluents by oxygen-distal fluorination for energy-dense Li metal battery

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年5月2日

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  • Xingmin Yu,
  • Yong Li,
  • Zhaofen Wang,
  • Haichen Huang,
  • Yaoyao Liu,
  • Lequan Deng,
  • Jun Zhan,
  • Xianglin Yin,
  • Haoying Qi,
  • Yushuang Yang,
  • Shuhua Wang,
  • Yuanhua Sang,
  • Daixin Ye,
  • Jian-Jun Wang,
  • Hong Liu,
  • Hao Chen

摘要

Enhancing cycling reversibility in high-energy-density lithium metal batteries necessitates precise management of electrolyte-derived electrochemical reactions at electrodes and interphases, yet recently developed localized high-concentration electrolytes suffer from limited tunability of these reactions for the non-solvation-participating nature of oxygen-proximal fluorinated diluents. Here we address this issue by synthesizing an oxygen-distal fluorinated di-2,2,3,3-tetrafluoropropoxyethane diluent whose molecular skeleton is strategically edited to position fluorine atoms distal to oxygen centers that attenuate electron-withdrawing effects at Li+-coordination sites, enabling: enhanced diluent/anion participation and reduced volatile solvents in solvation shells; atypical H-F bonding between diluent and solvent toward enhanced oxidation resistance; and promotion of diluent and salt-derived highly stable inorganic-rich interphase formation. This electrolyte achieves 99.8% Li plating/stripping Coulombic efficiency, 450 stable cycles in 4.5 V high-voltage Li || LiNi0.8Mn0.1Co0.1O2 cells, and 5.9-Ah, 504.6 Wh kg–1 (based on mass of all components including packaging) pouch cells that exhibits 0.053% per-cycle capacity decay. This work introduces oxygen-distal fluorination as a potential molecular skeleton editing strategy for stable energy-dense lithium metal batteries.