Polycation ionic liquid tailored PEO-based solid polymer electrolytes for high temperature lithium metal batteries

Poly(ethylene oxide) (PEO)-based polymer electrolytes are promising candidates for solid-state electrolytes in safer, next generation lithium metal batteries. Despite their benefits however, PEO-based electrolyte exhibits highly crystalline ethylene oxide chains that provide poor ionic conductivity and, thus severely limit its practical application. Here, we report the use of hydroxypropyl trimethylammonium bis(trifluoromethane) sulfonimide chitosan salt (HACC-TFSI), which is an amorphous poly(ionic liquid) based biomass chitosan derivative, as a modifier for PEO-based solid polymer electrolytes (SPEs) to address these deficiencies. Hybrid SPEs with HACC-TFSI display enlarged amorphous regions with enhanced ionic conductivity. Interactions between quaternary ammonium cations and TFSI− anions in hybrid SPEs are also found to promote dissociation between Li+ and TFSI−, which further increases ionic mobility. Moreover, the electrochemical stability, mechanical strength, and thermal stability of hybrid SPEs are collectively superior to blank SPEs without HACC-TFSI. LiFePO4/SPEs/Li full-cells assembled using 10wt% HACC-TFSI in PEO (10%HACC-TFSI/SPEs) electrolyte provide a capacity of 161.3 mAh g−1 and operate with excellent cycle performances at 0.2 C and 60 °C. Even when the temperature is increased to 150 °C, LiFePO4/SPEs/Li cells with 10%HACC-TFSI/SPEs still display remarkable cycle performance with 73% capacity retention after 100 cycles at 1 C rate.