This perspective reviews current strategies to decouple segmental motion and ionic conductivity for lithium polymer battery electrolytes, including an outlook for potential future improvements.

In this work, new gelled electrolytes were prepared based on a mixture containing phosphonium ionic liquid (IL) composed of trihexyl(tetradecyl)phosphonium cation combined with bis(trifluoromethane)sulfonimide [TFSI] counter anions and lithium salt, confined in a host network made from an epoxy prepolymer and amine hardener. We have demonstrated that the addition of electrolyte plays a key role on the kinetics of polymerization but also on the final properties of epoxy networks, especially thermal, thermo-mechanical, transport, and electrochemical properties. Thus, polymer electrolytes with excellent thermal stability (>300 °C) combined with good thermo-mechanical properties have been prepared. In addition, an ionic conductivity of 0.13 Ms·cm⁻¹ at 100 °C was reached. Its electrochemical stability was 3.95 V vs. Li⁰/Li⁺ and the assembled cell consisting in Li|LiFePO₄ exhibited stable cycle properties even after 30 cycles. These results highlight a promising gelled electrolyte for future lithium ion batteries.