Regulation of Outer Solvation Shell Toward Superior Low‐Temperature Aqueous Zinc‐Ion Batteries

Abstract Aqueous Zn‐ion batteries are well regarded among a next‐generation energy‐storage technology due to their low cost and high safety. However, the unstable stripping/plating process leading to severe dendrite growth under high current density and low temperature impede their practical application. Herein, it is demonstrated that the addition of 2‐propanol can regulate the outer solvation shell structure of Zn 2+ by replacing water molecules to establish a “eutectic solvation shell”, which provides strong affinity with the Zn (101) crystalline plane and fast desolvation kinetics during the plating process, rendering homogeneous Zn deposition without dendrite formation. As a result, the Zn anode exhibits promising cycle stability over 500 h under an elevated current density of 15 mA cm −2 and high depth of discharge of 51.2%. Furthermore, remarkable electrochemical performance is achieved in a 150 mAh Zn|V 2 O 5 pouch cell over 1000 cycles at low temperature of −20 °C. This work not only offers a new strategy to achieve excellent performance of aqueous Zn‐ion batteries under harsh conditions, but also reveals electrolyte structure designs that can be applied in related energy storage and conversion fields.