Construction of Bio‐inspired Film with Engineered Hydrophobicity to Boost Interfacial Reaction Kinetics of Aqueous Zinc–Ion Batteries

Abstract Aqueous zinc–ion batteries typically suffer from sluggish interfacial reaction kinetics and drastic cathode dissolution owing to the desolvation process of hydrated Zn 2+ and continual adsorption/desorption behavior of water molecules, respectively. To address these obstacles, a bio‐inspired approach, which exploits the moderate metabolic energy of cell systems and the amphiphilic nature of plasma membranes, is employed to construct a bio‐inspired hydrophobic conductive poly(3,4‐ethylenedioxythiophene) film decorating α‐MnO 2 cathode. Like plasma membranes, the bio‐inspired film can “selectively” boost Zn 2+ migration with a lower energy barrier and maintain the integrity of the entire cathode. Electrochemical reaction kinetics analysis and theoretical calculations reveal that the bio‐inspired film can significantly improve the electrical conductivity of the electrode, endow the cathode–electrolyte interface with engineered hydrophobicity, and enhance the desolvation behavior of hydrated Zn 2+ . This results in an enhanced ion diffusion rate and minimized cathode dissolution, thereby boosting the overall interfacial reaction kinetics and cathode stability. Owing to these intriguing merits, the composite cathode can demonstrate remarkable cycling stability and rate performance in comparison with the pristine MnO 2 cathode. Based on the bio‐inspired design philosophy, this work can provide a novel insight for future research on promoting the interfacial reaction kinetics and electrode stability for various battery systems.