Anionic Chemistry Modulation Enabled Environmental Self‐Charging Aqueous Zinc Batteries: The Case of Carbonate Ions

Abstract Anionic chemistry modulation represents a promising avenue to enhance the electrochemical performance and unlock versatile applications in cutting‐edge energy storage devices. Herein, we propose a methodology that involves anionic chemistry of carbonate anions to tailor the electrochemical oxidation‐reduction reactions of bismuth (Bi) electrodes, where the conversion energy barrier for Bi (0) to Bi (III) has been significantly reduced, endowing anionic full batteries with enhanced electrochemical kinetics and chemical self‐charging property. The elaborately designed batteries with an air‐switch demonstrate rapid self‐recharging capabilities, recovering over 80 % of the electrochemical full charging capacity within a remarkably short timeframe of 1 hour and achieving a cumulative self‐charging capacity of 5 Ah g −1 . The aqueous self‐charging battery strategy induced by carbonate anion, as proposed in this study, holds the potential for extending to various anionic systems, including seawater‐based Cl − ion batteries. This work offers a universal framework for advancing next‐generation multi‐functional power sources.