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<p>The instability of lithium salts within the electrolyte has consistently posed a significant challenge to next-generation lithium-ion batteries. The most commercialized lithium hexafluorophosphate (LiPF<sub>6</sub>) suffers from ligand abstraction, causing excessive formation of erosive HF at elevated temperatures. Another promising salt of lithium difluoro(oxalato)borate (LiDFOB), featuring hydrophilic/lithiophilic carbonyl groups, possesses high moisture sensitivity and insufficient dissociation in electrolytes. Herein, we propose an anion-skeleton editing strategy that increases the fluoride ion affinity of the parent Lewis acid while reducing its interaction with H<sup>+</sup>/Li<sup>+</sup> by replacing the carbonyl groups in DFOB<sup>-</sup> anion with hydrophobic/lithiophobic -CF<sub>3</sub> groups. The lithium salt alternative, lithium 2,2-difluoro-4,4,5,5-tetrakis(trifluoromethyl)−1,3,2-dioxaborolan-2-uide (LiDFTFB), has been successfully synthesized and serves as a well-balanced salt in terms of moisture stability, thermal stability, electrochemical stability, ionic conductivity, solubility, and aluminum foil passivation, outperforming LiPF<sub>6</sub> and LiDFOB. Even at an elevated temperature of 50 °C, LiDFTFB endows 1 Ah graphite | |LiNi<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub> pouch cells with enhanced cycling stability (81.7% retention after 650 cycles, 0.5 C charge and 0.5 C discharge, 1 C = 200 mA g<sup>-1</sup>). This work emphasizes the critical importance of strategically modulating anion chemistries to promote the development of the next-generation lithium-ion batteries.</p>

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Tailored electrolyte salt anion chemistry for enhanced high-nickel lithium-ion batteries

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年12月11日

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  • Shitao Wang,
  • Lixin Qiao,
  • Jinlong Li,
  • Shu Zhang,
  • Shenghang Zhang,
  • Xiangchun Zhuang,
  • Yu Zhao,
  • Xiaofan Du,
  • Bin Xie,
  • Kai Chen,
  • Renteng Du,
  • Qingrui Kong,
  • Zhaolin Lv,
  • Zili Cui,
  • Shanmu Dong,
  • Gaojie Xu,
  • Michel Armand,
  • Guanglei Cui

摘要

The instability of lithium salts within the electrolyte has consistently posed a significant challenge to next-generation lithium-ion batteries. The most commercialized lithium hexafluorophosphate (LiPF6) suffers from ligand abstraction, causing excessive formation of erosive HF at elevated temperatures. Another promising salt of lithium difluoro(oxalato)borate (LiDFOB), featuring hydrophilic/lithiophilic carbonyl groups, possesses high moisture sensitivity and insufficient dissociation in electrolytes. Herein, we propose an anion-skeleton editing strategy that increases the fluoride ion affinity of the parent Lewis acid while reducing its interaction with H+/Li+ by replacing the carbonyl groups in DFOB- anion with hydrophobic/lithiophobic -CF3 groups. The lithium salt alternative, lithium 2,2-difluoro-4,4,5,5-tetrakis(trifluoromethyl)−1,3,2-dioxaborolan-2-uide (LiDFTFB), has been successfully synthesized and serves as a well-balanced salt in terms of moisture stability, thermal stability, electrochemical stability, ionic conductivity, solubility, and aluminum foil passivation, outperforming LiPF6 and LiDFOB. Even at an elevated temperature of 50 °C, LiDFTFB endows 1 Ah graphite | |LiNi0.8Mn0.1Co0.1O2 pouch cells with enhanced cycling stability (81.7% retention after 650 cycles, 0.5 C charge and 0.5 C discharge, 1 C = 200 mA g-1). This work emphasizes the critical importance of strategically modulating anion chemistries to promote the development of the next-generation lithium-ion batteries.