Thermoresponsive Electrolytes for Safe Lithium-Metal Batteries

Exploring advanced strategies in alleviating the thermal runaway of lithium-metal batteries (LMBs) is critically essential. Herein, a novel electrolyte system with thermoresponsive characteristics is designed to largely enhance the thermal safety of 1.0 Ah LMBs. Specifically, vinyl carbonate (VC) with azodiisobutyronitrile is introduced as a thermoresponsive solvent to boost the thermal stability of both the solid electrolyte interphase (SEI) and electrolyte. First, abundant poly(VC) is formed in SEI with thermoresponsive electrolyte, which is more thermally stable against lithium hexafluorophosphate compared to the inorganic components widely acquired in routine electrolyte. This increases the critical temperature for thermal safety (the beginning temperature of obvious self-heating) from 71.5 to 137.4 degrees C. The remained VC solvents can be polymerized into poly(VC) as the battery temperature abnormally increases. The poly(VC) can not only afford as a barrier to prevent the direct contact between electrodes, but also immobilize the free liquid solvents, thereby reducing the exothermic reactions between electrodes and electrolytes. Consequently, the internal-short-circuit temperature and ignition point temperature (the starting temperature of thermal runaway) of LMBs are largely increased from 126.3 and 100.3 degrees C to 176.5 and 203.6 degrees C. This work provides novel insights for pursuing thermally stable LMBs with the addition of various thermoresponsive solvents in commercial electrolytes.

Automated summary

A novel electrolyte system with thermoresponsive characteristics is designed to enhance the thermal safety of lithium-metal batteries. The introduction of VC and azodiisobutyronitrile results in the formation of abundant poly(VC) in the solid electrolyte interphase, which improves the thermal stability of SEI. This electrolyte not only prevents direct contact between electrodes, but also reduces exothermic reactions between electrodes and electrolytes, thus increasing the thermal safety of the batteries.