Supramolecular Self-Assembly Regulated Double-Network Ionic Gel Electrolyte for Advanced Electrochromic Device

Ionic gels represent a promising electrolyte platform for electrochromic devices owing to their intrinsic ionic conductivity and safety. However, achieving mechanical robustness and interfacial adhesion without sacrificing ionic conductivity remains a significant challenge. In this work, we present a supramolecular-polymer double-network (SP-DN) ionic gel electrolyte, in which a supramolecular network formed through the self-assembly of 1,3:2,4-dibenzylidene sorbitol synergistically interacts with a covalently cross-linked polymer network. The SP-DN ionic gel synergizes superior mechanical strength and robust interfacial adhesion with high ionic conductivity and optical transparency. Electrochromic devices fabricated with this ionic gel electrolyte show rapid switching dynamics, high coloration efficiency, and robust stability over 2000 cycles. Moreover, electrochromic devices fabricated on ITO-poly(ethylene terephthalate) substrates retain 90.6% of their initial optical contrast after 1000 bending cycles, underscoring the potential of the SP-DN ionic gel for flexible applications.