ABSTRACT Wide‐temperature and high‐voltage environments impose unprecedented demands on electrolyte stability, where conventional systems tend to fail due to severe by‐products generation and cathode‐electrolyte interphase (CEI) / solid electrolyte interface (SEI) corrosion. Herein, a molecularly engineered cross‐linker (pentafluorobutyl acrylate, PFPA) is proposed to achieve rapid self‐repairing of CEI/SEI through sequential fluorine release. It is revealed that the grafted pentafluorophenyl groups of PFPA can suppress harmful hydrolysis preventatively and increase the Li + transference number by implanting PF 6 − , and achieve the construction and continuous self‐repairing of LiF‐rich CEI/SEI. As a result, the cells incorporating modified electrolytes (GPE‐F) exhibit excellent electrochemical performance under a high cut‐off voltage (∼4.7 V) and a wide temperature range (‐20∼70°C). The NCM811||GPE‐F||Li pouch cell with 403.6 Wh kg −1 delivers a high‐capacity retention of 91.3% after 380 cycles, and the NCM811||GPE‐F||Gr pouch cell with 265.5 Wh kg −1 can be stably cycled for over 2000 cycles. The industrial viability is further demonstrated in high‐capacity (11.1 Ah), high‐energy‐density pouch cells (544.3 Wh kg −1 ). This work provides a novel and promising pathway for the development of multi‐system compatible gel polymer electrolytes, particularly for their application in complex and harsh operating environments.
Peng et al. (2026) studied this question.