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<p>Ion association in highly concentrated electrolytes and localized highly concentrated electrolytes facilitates solid electrolyte interphase formation but compromises the thermal stability. Here we investigated the thermal behaviours of 20 electrolytes and uncovered that ion association lowers exothermic onset temperature by ~94 °C. To enhance the thermal stability without impairing solid electrolyte interphase formation, we developed a solvent-relay strategy that promotes ion association at ambient temperature while inducing dissociation at elevated temperatures. This approach enabled 4.5-V graphite-NCM811 pouch cells (1.1 Ah) to deliver 1,000 cycles under 0.45 C over 4,100 h with ~81.9% capacity retention and exceptional thermal safety, with a temperature rise lower than 3.5 °C during nail penetration, compared with 555.2 °C for commercial carbonate-based electrolytes. These findings elucidate the pivotal role of ion association in thermal runaway and offer a viable strategy to simultaneously achieve long cycle life, high-voltage operation and enhanced safety in ampere-hour-scale lithium-ion batteries.</p>

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Designing safe and long-life lithium-ion batteries via a solvent-relay strategy

  • 期刊论文

  • 发表日期：

    2025年10月17日

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  • Yue Sun,
  • Changjian Zuo,
  • Huwei Wang,
  • Liwei Jiang,
  • Wanwan Wang,
  • Jing Xie,
  • Yi-Chun Lu

摘要

Ion association in highly concentrated electrolytes and localized highly concentrated electrolytes facilitates solid electrolyte interphase formation but compromises the thermal stability. Here we investigated the thermal behaviours of 20 electrolytes and uncovered that ion association lowers exothermic onset temperature by ~94 °C. To enhance the thermal stability without impairing solid electrolyte interphase formation, we developed a solvent-relay strategy that promotes ion association at ambient temperature while inducing dissociation at elevated temperatures. This approach enabled 4.5-V graphite-NCM811 pouch cells (1.1 Ah) to deliver 1,000 cycles under 0.45 C over 4,100 h with ~81.9% capacity retention and exceptional thermal safety, with a temperature rise lower than 3.5 °C during nail penetration, compared with 555.2 °C for commercial carbonate-based electrolytes. These findings elucidate the pivotal role of ion association in thermal runaway and offer a viable strategy to simultaneously achieve long cycle life, high-voltage operation and enhanced safety in ampere-hour-scale lithium-ion batteries.