Regulating Interfacial Ion Adsorption for Smooth and Durable Zinc Cycling at High Area Capacity

Reversible and dendrite‐free zinc (Zn) circulation is essential for longevous aqueous zinc‐ion batteries (ZIBs) and greatly impacted by the property of Zn interface and electrolyte, especially when confronted with high current density and large area capacity. Herein, a hierarchical Zn interface is constructed by the preferential anion surfactant adsorption and reaction, and assists to reduce the interfacial energy and side reactions for enhanced diffusion kinetics and reversibility during Zn plating/stripping. Thus, highly reversible and smooth Zn anodes are achieved with a long‐term stability of 5500 h at 1 mA cm−2/1 mAh cm−2, an impressive rate up to 40 mA cm−2 for 10 mAh cm−2 and a large cumulative plating capacity of 4.45 Ah cm−2 at 10 mA cm−2 in Zn symmetric cells. Even under a high depth of discharge of 60% (5.85/7.65 mAh cm−2), Zn symmetric batteries can still maintain ca. 800 h's life. The proposed countermeasure has also proved to be valid in prolonging the lifespan and stability of Zn‐MnO2 full batteries at both low and high cycling current densities. An interfacial regulation strategy of preferential adsorption via anionic surfactants, 2‐acrylamide‐2‐methylpropanesulfonic (AMPS), is proposed to reduce side reactions and enhance the diffusion kinetics of zinc‐ion at the zinc/electrolyte interface, thereby achieving highly reversible and flat zinc anode at large area capacity and depth of discharge.