Bioinspired Tough Solid-State Electrolyte for Flexible Ultralong-Life Zinc–Air Battery

Manufacturing advanced solid-state electrolytes (SSEs) for flexible rechargeable batteries becomes increasingly important but remains grand challenge. The sophisticated structure of robust animal dermis and good water-retention of plant cell in nature grant germane inspirations for designing high-performance SSEs. Herein, tough bioinspired SSEs with intrinsic hydroxide ion (OH⁻) conduction are constructed by in situ formation of OH⁻ conductive ionomer network within a hollow-polymeric-microcapsule-decorated hydrogel polymer network. By virtue of the bioinspired design and dynamic dual-penetrating network structure, the bioinspired SSEs simultaneously obtain mechanical robustness with 1800% stretchability, good water uptake of 107 g g⁻¹ and water retention, and superhigh ion conductivity of 215 mS cm⁻¹. The nanostructure of bioinspired SSE and related ion-conduction mechanism are revealed and visualized by molecular dynamics simulation, where plenty of compact and superfast ion-transport channels are constructed, contributing to superhigh ion conductivity. As a result, the flexible solid-state zinc–air batteries assembled with bioinspired SSEs witness high power density of 148 mW cm⁻², specific capacity of 758 mAh g⁻¹ and ultralong cycling stability of 320 h as well as outstanding flexibility. The bioinspired methodology and deep insight of ion-conduction mechanism will shed light on the design of advanced SSEs for flexible energy conversion and storage systems.