Tough Hydrogel Electrolytes for Anti‐Freezing Zinc‐Ion Batteries

As the soaring demand for energy storage continues to grow, batteries that can cope with extreme conditions are highly desired. Yet, existing battery materials are limited by weak mechanical properties and freeze-vulnerability, prohibiting safe energy storage in devices that are exposed to low temperature and unusual mechanical impacts. Herein, a fabrication method harnessing the synergistic effect of co-nonsolvency and "salting-out" that can produce poly(vinyl alcohol) hydrogel electrolytes with unique open-cell porous structures, composed of strongly aggregated polymer chains, and containing disrupted hydrogen bonds among free water molecules, is introduced. The hydrogel electrolyte simultaneously combines high strength (tensile strength 15.6 MPa), freeze-tolerance (< -77 °C), high mass transport (10× lower overpotential), and dendrite and parasitic reactions suppression for stable performance (30 000 cycles). The high generality of this method is further demonstrated with poly(N-isopropylacrylamide) and poly(N-tertbutylacrylamide-co-acrylamide) hydrogels. This work takes a further step toward flexible battery development for harsh environments.