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<p>Lithium metal batteries face serious safety challenges caused by flammable organic electrolytes and the growth of lithium dendrite. Trimethyl phosphate (TMP) is a promising alternative for flammable carbonate electrolyte solvents owing to its nonflammable nature. But the low-concentration TMP-based electrolyte is unstable with the lithium metal anode. Here, a TMP-contained quasi-solid electrolyte (PIQSE) with porous polyimide (PI) as supporting skeleton is designed. The cross-linking structure generated by UV curing in PIQSE can lock the reactive TMP solvent to reduce its contact with Li metal. Besides, the PI supporting skeleton with high-temperature resistance can significantly enhance the thermal stability of PIQSE. The combination of PI and TMP prompts the high ionic conductivity and excellent nonflammability of PIQSE. The LiFePO<sub>4</sub>/Li cell using PIQSE shows superior electrochemical performance in a wide temperature range from −10 to 60&#xa0;°C. Furthermore, the cells with high-voltage cathode of LiNi<sub>0.6</sub>Co<sub>0.2</sub>Mn<sub>0.2</sub>O<sub>2</sub> (NCM622) were matched with PIQSE exhibit good cyclic and rate performance. The NCM622/PIQSE/Li pouch cell was also fabricated. It exhibits a high discharge capacity of 182.9 mAh·g<sup>−1</sup>, and can stably light up LEDs after folding and shearing tests, demonstrating broad prospects for highly safe energy storage applications.</p> Graphical abstract <p></p>

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Non-flammable and stable phosphate quasi-solid electrolyte with low salt concentration for lithium metal batteries

  • 期刊论文

  • 发表日期：

    2025年2月28日

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  • Man-Ni Li,
  • Fei Shen,
  • Kai-Ming Wang,
  • Zhe Zhang,
  • Xiao-Gang Han

摘要

Lithium metal batteries face serious safety challenges caused by flammable organic electrolytes and the growth of lithium dendrite. Trimethyl phosphate (TMP) is a promising alternative for flammable carbonate electrolyte solvents owing to its nonflammable nature. But the low-concentration TMP-based electrolyte is unstable with the lithium metal anode. Here, a TMP-contained quasi-solid electrolyte (PIQSE) with porous polyimide (PI) as supporting skeleton is designed. The cross-linking structure generated by UV curing in PIQSE can lock the reactive TMP solvent to reduce its contact with Li metal. Besides, the PI supporting skeleton with high-temperature resistance can significantly enhance the thermal stability of PIQSE. The combination of PI and TMP prompts the high ionic conductivity and excellent nonflammability of PIQSE. The LiFePO4/Li cell using PIQSE shows superior electrochemical performance in a wide temperature range from −10 to 60 °C. Furthermore, the cells with high-voltage cathode of LiNi0.6Co0.2Mn0.2O2 (NCM622) were matched with PIQSE exhibit good cyclic and rate performance. The NCM622/PIQSE/Li pouch cell was also fabricated. It exhibits a high discharge capacity of 182.9 mAh·g−1, and can stably light up LEDs after folding and shearing tests, demonstrating broad prospects for highly safe energy storage applications.

Graphical abstract