Gel electrolyte membranes derived from co-continuous polymer blends

Polymer gel electrolyte membranes were prepared by first casting films of poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF–HFP), lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) salt, and poly(ethylene glycol) (PEG) monomethacrylate and dimethacrylate macromonomers. Polymerization of the macromonomers initiated by UV-irradiation then generated solid films having phase-separated morphologies with a microporous PVDF–HFP phase embedded in PEG-grafted polymethacrylates. Gel electrolyte membranes were finally prepared by allowing the films to take up solutions of LiTFSI in γ-butyrolactone (γ-BL). The PEG-grafted polymethacrylate in the membranes was found to host the largest part of the liquid electrolyte, giving rise to a highly swollen ionic conductive phase. Results by FTIR spectroscopy showed that the Li+ ions preferentially interacted with the ether oxygens of the PEG chains. The properties of the membranes were studied as a function of the ratio of PVDF–HFP to PEG-grafted polymethacrylate, as well as the degree of crosslinking, LiTFSI concentration, and liquid electrolyte content. The self-supporting and elastic gel membranes had ionic conductivities of 10−3 S cm−1 and a mechanical storage modulus in the range of 2.5 MPa in the tension mode at room temperature. Variation of the salt concentration showed the greatest effect on the membrane properties.