Dynamic Interfacial Alloying for Highly Reversible Zinc Anodes

Abstract Rechargeable aqueous zinc batteries offer compelling advantages for large‐scale energy storage through cost‐effectiveness and intrinsic safety, yet suffer from poor reversibility due to uncontrolled dendrite growth and parasitic reactions. To address this challenge, an interfacial layer is designed to enables dynamic alloying on the Zn surface, thereby sustaining the supply of zincophilic sites and preventing failures arising from the coverage of zincophilic sites by deposited Zn. The alloy guides Zn to selectively deposit along the (002) crystal plane, which effectively inhibits dendrite formation and stabilizes Zn/electrolyte interface. In addition, it facilitates anode self‐healing through preferential deposition at defect sites. As a result, symmetric cells equipped with the interface layer demonstrate stable cycling for over 600 h at a high current density of 20 mA cm ⁻² , corresponding to an accumulated areal capacity exceeding 6 Ah cm ⁻² . The ZnllNH ₄ ⁺ ‐V ₂ O ₅ cell delivers an initial areal discharge capacity of 3.5 mAh cm ⁻² and operates over 1000 cycles at 200 mA g ⁻¹ . This performance underscores the effectiveness of the dynamic interfacial alloying strategy in achieving durable Zn anode performance under rigorous electrochemical conditions.