Xylose- and Nucleoside-Based Polymers via Thiol-ene Polymerization toward Sugar-Derived Solid Polymer Electrolytes

A series of copolymers have been prepared via thiol-ene polymerization of bioderived alpha,omega-unsaturated diene monomers with dithiols toward application as solid polymer electrolytes (SPEs) for Li+-ion conduction. Amorphous polyesters and polyethers with low T-g's (-31 to -11 degrees C) were first prepared from xylose-based monomers (with varying lengths of fatty acid moiety) and 2,2 '-(ethylenedioxy)diethanethiol (EDT). Cross-linking by incorporation of a trifunctional monomer also produced a series of SPEs with ionic conductivities up to 2.2 x 10(-5) S cm(-1) at 60 degrees C and electrochemical stability up to 5.08 V, a significant improvement over previous xylose-derived materials. Furthermore, a series of copolymers bearing nucleoside moieties were prepared to exploit the complementary base-pairing interaction of nucleobases. Flexible, transparent, and reprocessable SPE films were thus prepared with improved ionic conductivity (up to 1.5 x 10(-4) S cm(-1) at 60 degrees C), hydrolytic degradability, and potential self-healing capabilities.