Investigating polypropylene-poly(ethylene oxide)-polypropylene triblock copolymers as solid polymer electrolytes for lithium batteries

•Synthesized syndiotactic polypropylene-poly(ethylene oxide) triblock copolymers•Solid polymer electrolytes (SPEs) of these copolymers and LiTFSI were prepared•These SPEs contained a semi-crystalline block as the mechanically reinforced agent•Thermal properties, ionic conductivity, and self-assembly of the SPEs are reported•An unusual ionic conductivity trend was observed for these SPEs

Syndiotactic polypropylene-b-poly(ethylene oxide)-b-syndiotactic polypropylene (PEOP) triblock copolymers were synthesized and solid polymer electrolytes were prepared by mixing with lithium bis(trifluoromethane)sulfonimide (LiTFSI) salt. PEOP formed strongly-segregated morphologies in the absence and presence of LiTFSI. LiTFSI inhibited poly(ethylene oxide) crystallization without affecting polypropylene crystallinity. The conductivity exhibited a non-monotonic dependence on molecular weight (Mn) with a maximum near 20 kg/mol. In contrast, polystyrene-b-poly(ethylene oxide) electrolytes exhibit conductivity increasing monotonically with Mn, up to a plateau in the high-Mn limit. This suggests that non-conducting semi-crystalline microphases interfere with conducting pathways, while non-conducting amorphous microphases formed well-connected conducting pathways.