Thermally Reprocessable Self-Healing Single-Ion Conducting Polymer Electrolytes

Abstract

Self-healing polymer electrolytes are essential for overcoming the limitations of liquid and solid electrolytes by offering superior mechanical robustness, enhanced safety, and repeated processability. Herein, we present thermally reprocessable and self-healing thermosets for solid polymer electrolytes using sulfonylimide-based anionic monomers and thermo-reversible Diels−Alder chemistry. Six different types of linear copolymers are synthesized by varying the chemical structures of furancontaining monomers and the proportion of electrolytic components. Then, bismaleimide cross-linkers are introduced to form thermally reversible cross-linked networks. We investigate the effect of the comonomer ratio and monomer structure on the thermomechanical and electrochemical properties of these polymers. Furthermore, we evaluate the mechanical and ion conducting properties after up to 30 thermal reprocessing cycles. Our findings demonstrate the potential of these thermosets as promising candidates for high-performance solid polymer electrolytes in lithium-ion batteries.

Polymer design for solid-state batteries and wearable electronics

“…Despite the relatively low ionic conductivities (0.07 mS cm −1 at 80 °C), the Diels–Alder adduct formed between the furan and maleimide moieties could be thermally reversed at 140 °C up to 30× to give polymers of comparable conductivity and mechanical robustness. 139 Thus, the inclusion of dynamic covalent linkages is a promising strategy towards more (re)processable and toughened SPEs – potentially robust enough to suppress Li dendrite growth. They may also pave the way to depolymerisable and/or recyclable electrolytes.…”