Thermally Reprocessable Self-Healing Single-Ion Conducting Polymer Electrolytes

Self-healing polymer electrolytes are essential for overcomingthe limitations of liquid and solid electrolytes by offering superiormechanical robustness, enhanced safety, and repeated processability.Herein, we present thermally reprocessable and self-healing thermosetsfor solid polymer electrolytes using sulfonylimide-based anionic monomersand thermo-reversible Diels-Alder chemistry. Six differenttypes of linear copolymers are synthesized by varying the chemicalstructures of furan-containing monomers and the proportion of electrolyticcomponents. Then, bismaleimide cross-linkers are introduced to formthermally reversible cross-linked networks. We investigate the effectof the comonomer ratio and monomer structure on the thermomechanicaland electrochemical properties of these polymers. Furthermore, weevaluate the mechanical and ion conducting properties after up to30 thermal reprocessing cycles. Our findings demonstrate the potentialof these thermosets as promising candidates for high-performance solidpolymer electrolytes in lithium-ion batteries.