Thermal-Gated Polymer Electrolytes for Smart Zinc-Ion Batteries

Smart self-protection is essential for addressing safety issues of energy-storage devices. However, conventional strategies based on sol-gel transition electrolytes often suffer from unstable self-recovery performance. Herein, smart separators based on thermal-gated poly(N-isopropylacrylamide) (PNIPAM) hydrogel electrolytes were developed for rechargeable zinc-ion batteries (ZIBs). Such PNIPAM-based separators not only display a pore structure evolution from opened to closed states, but also exhibit a surface wettability transition from hydrophilic to hydrophobic behaviors when the temperature rises. This behavior can suppress the migration of electrolyte ions across the separators, realizing the self-protection of ZIBs at high temperatures. Furthermore, the thermal-gated behavior is highly reversible, even after multiple heating/cooling cycles, because of the reversibility of temperature-dependent structural evolution and hydrophilic/hydrophobic transition. This work will pave the way for designing thermal-responsive energy-storage devices with safe and controlled energy delivery.