Cation and Anion Modulation Strategies toward Ideal Zinc Artificial Interface

Abstract Aqueous zinc‐ion batteries (ZIBs) stand out as promising next‐generation energy storage systems. However, the Zn anode failure caused by the unstable Zn/electrolyte interface hinders their practical applications. Constructing artificial layer on the Zn surface provides an effective method to optimize the interfacial stability and mitigate the issues, while most of the current investigations put emphasis on the discussion of Zn 2+ and H 2 O regulation, we notice that the anions and hydrogen evolution reaction (HER) intermediates also play a crucial role in the occurrence of side reactions, thus a comprehensive evaluation of interfacial modulation strategies regarding all the different ion species in ZIBs system is helpful for developing advanced artificial interface. Herein, this work systematically reviews the achievements about cation and anion modulation strategies for stabilizing Zn/electrolyte interface and emphasizes on the relationship between the material properties and ionic regulation mechanisms for the first time, aiming to provide an unprecedented design reference. Furthermore, some noteworthy points and perspectives are proposed, which has guiding significance for the realization of high‐performance and multi‐level regulated Zn anode.