<p>Short circuits in lithium metal batteries caused by separator failure at elevated temperatures present a critical thermal safety challenge. Smart, temperature-responsive materials offer a promising way to prevent short circuits, yet practical systems with sufficiently fast response times have not been realized. Here we propose a thermo-responsive electrolyte that undergoes a rapid liquid-to-solid phase transition upon heating, offering a highly effective strategy to enhance lithium metal battery safety. The electrolyte leverages LiPF<sub>6</sub> to initiate cationic polymerization, enabling solidification within seconds at a temperature threshold near the separator’s melting point. This fast phase change forms an effective heat shield that prevents internal short circuits and thermal runaway. Demonstrated in LiFePO<sub>4</sub>||Li pouch cells, the electrolyte ensures stable operation up to 90 °C and completely suppresses thermal runaway. Notably, the transition temperature can be tuned between 100 °C and 150 °C, allowing compatibility with various commercial separators. This ultrafast thermo-responsive electrolyte offers a pathway towards the design of intrinsically safe lithium metal batteries.</p>

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Ultrafast thermo-responsive electrolyte for enhanced safety in lithium metal batteries

  • Chao Yang,
  • Wenxi Hu,
  • Mengting Zheng,
  • Xing Zhou,
  • Xiaowei Liu,
  • Jingting Yang,
  • Dawei Xu,
  • Meilong Wang,
  • Youcai Zhang,
  • Wen Chen,
  • Jun Lu,
  • Ya You

摘要

Short circuits in lithium metal batteries caused by separator failure at elevated temperatures present a critical thermal safety challenge. Smart, temperature-responsive materials offer a promising way to prevent short circuits, yet practical systems with sufficiently fast response times have not been realized. Here we propose a thermo-responsive electrolyte that undergoes a rapid liquid-to-solid phase transition upon heating, offering a highly effective strategy to enhance lithium metal battery safety. The electrolyte leverages LiPF6 to initiate cationic polymerization, enabling solidification within seconds at a temperature threshold near the separator’s melting point. This fast phase change forms an effective heat shield that prevents internal short circuits and thermal runaway. Demonstrated in LiFePO4||Li pouch cells, the electrolyte ensures stable operation up to 90 °C and completely suppresses thermal runaway. Notably, the transition temperature can be tuned between 100 °C and 150 °C, allowing compatibility with various commercial separators. This ultrafast thermo-responsive electrolyte offers a pathway towards the design of intrinsically safe lithium metal batteries.