Deep eutectic electrolytes (DEEs) provide a safe solution
for high-temperature
batteries. While promising, the DEEs/electrode interphase chemistry
and the underlying temperature mechanism remain unclear. Herein, the
DEE is formulated with succinonitrile (SCL) and lithium bis(fluorosulfonyl)
imide (LiFSI) to promote the mesocarbon microbead (MCMB) anode in
high-temperature Li-ion batteries. The temperature-sensitive mechanism
of solid electrolyte interphase (SEI) evolution on the MCMB is deciphered,
the core of which is temperature-regulated solvation chemistry. Specifically,
high temperature can result in the enhanced interaction between Li+ and FSI– anions in the solvation structure,
thus elevating the LiF content in the SEI. Due to the synergy of DEE
(featuring rapid ion conduction and thermal stability) and high-temperature
optimized interphase, MCMB/Li and LiFePO4/MCMB cells exhibit
improved cycling stability at high temperature. This work promotes
a fundamental understanding of the intrinsic relationship between
the temperature factor and SEI evolution, illuminating the future
of DEEs in high-temperature batteries.