Interfacial Alloying‐Induced Optimization of Zn 2+ Diffusion and Atomic Migration for Stable Aqueous Zn Batteries

Abstract Dendrite formation and corrosion issues of zinc anode hinder the practical application of aqueous rechargeable zinc‐ion batteries (AZIBs). Controlling the interfacial morphology during electrochemical process is critical for mitigating dendrite growth and corrosion issues in zinc electrodeposition. Herein, taking gallium (Ga) and indium (In) as the model system, three types of alloy‐coated zinc anodes, namely GaInZn‐coated Zn (GIZ), InZn‐coated Zn (IZ), and GaZn‐coated Zn (GZ) are designed. This work systematically investigates the morphology evolution and corrosion behavior of pure Zn and coated Zn anodes during the electrodeposition process, aiming to reveal the correlation between electrochemical behavior and deposition substrates. The design of alloy‐coated Zn anode provides novel insights into zinc‐ion diffusion in the electrolyte, nucleation on the alloy surfaces, and atomic diffusion behavior within the alloy phase. Specifically, the GIZ alloy phase regulates the migration of zinc ions, promotes zincophilic ion deposition, and suppresses anode corrosion tendency. Owing to preferential nucleation and enhanced corrosion resistance, the modified symmetric cell demonstrates stable operation for over 3000 h (>4 months) at 1 mA cm −2 with a capacity of 1 mAh cm −2 .