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<p>The next-generation of lithium metal batteries urgently require electrolytes that simultaneously possess low-cost, high-safety, wide-temperature operating range, high electrochemical stability and good electrode-electrolyte interphases formation ability. Here we present a flame-retardant electrolyte by introducing electrochemically-inert and weakly coordinating dichloroalkane diluents in triethyl phosphate-based high-concentration electrolyte. We systematically investigate the effects of dichloroalkane diluents with diverse carbon chain lengths on the Li<sup>+</sup> solvation structure, redox behavior, and lithium metal interfacial chemistry in the electrolyte. Consequently, 1,3-dichloropropane, which shows the favorable electrochemical inertness, weakly coordinating ability and wide liquid temperature range (−99 to +120 °C), is chosen as an ideal diluent in electrolyte to form robust anions-derived inorganic-rich electrode-electrolyte interphases on electrodes and improve the Li<sup>+</sup> transport/de-solvation capability. The developed electrolyte exhibits significant improvement in safety, cycling stability, rate capability and wide temperature operation capability of high-voltage lithium metal batteries. Particularly, the practical Li (50 μm)||LiNi<sub>0.83</sub>Co<sub>0.12</sub>Mn<sub>0.05</sub>O<sub>2</sub> (NCM83, 5.6 mAh cm<sup>−2</sup>) pouch cells exhibit stable cycling performance over 100 cycles with a high capacity retention rate of 94.1% at 0.1 C charge/0.2 C discharge under 25 °C, and deliver a promising application potential within a broad temperature range of −60 to +60 °C.</p>

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Flame-retardant electrolytes with electrochemically-inert and weakly coordinating dichloroalkane diluents for practical lithium metal batteries

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年11月19日

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  • Zhicheng Wang,
  • Haifeng Tu,
  • Xingdong Ma,
  • Suwan Lu,
  • Guirong Su,
  • Yiwen Gao,
  • Jiangyan Xue,
  • Lingwang Liu,
  • Xu Yao,
  • Kun Liang,
  • Ke Wang,
  • Fengrui Zhang,
  • Zhifeng Qin,
  • Jieyun Zheng,
  • Qing Wang,
  • Jingjing Xu,
  • Liquan Chen,
  • Hong Li,
  • Xiaodong Wu

摘要

The next-generation of lithium metal batteries urgently require electrolytes that simultaneously possess low-cost, high-safety, wide-temperature operating range, high electrochemical stability and good electrode-electrolyte interphases formation ability. Here we present a flame-retardant electrolyte by introducing electrochemically-inert and weakly coordinating dichloroalkane diluents in triethyl phosphate-based high-concentration electrolyte. We systematically investigate the effects of dichloroalkane diluents with diverse carbon chain lengths on the Li+ solvation structure, redox behavior, and lithium metal interfacial chemistry in the electrolyte. Consequently, 1,3-dichloropropane, which shows the favorable electrochemical inertness, weakly coordinating ability and wide liquid temperature range (−99 to +120 °C), is chosen as an ideal diluent in electrolyte to form robust anions-derived inorganic-rich electrode-electrolyte interphases on electrodes and improve the Li+ transport/de-solvation capability. The developed electrolyte exhibits significant improvement in safety, cycling stability, rate capability and wide temperature operation capability of high-voltage lithium metal batteries. Particularly, the practical Li (50 μm)||LiNi0.83Co0.12Mn0.05O2 (NCM83, 5.6 mAh cm−2) pouch cells exhibit stable cycling performance over 100 cycles with a high capacity retention rate of 94.1% at 0.1 C charge/0.2 C discharge under 25 °C, and deliver a promising application potential within a broad temperature range of −60 to +60 °C.