Mercaptosilane Engineered Interface with Surface‐Preferred Crystal Plane for High‐Performance Zn Anode

Abstract Zn‐ion battery (ZIB) has drawn huge attentions as a prospective energy storage system for the next generation, but dendrite and side reaction issues related to Zn have limited their potential applications. Here, a combined approach involving the modification of surface texture and the implementation of a passivation layer is proposed to tackle the problem. A zinc‐silane composite layer is coated on (002)‐preferred Zn (ZSi@Zn) by selective acid etching, concomitant with the hydrolysis of Mercaptosilane. The preferred (002) crystal plane, in conjunction with the zinc‐silane composite layer, leads in integrated interfacial transport and deposition control. As a result, the ZSi@Zn electrode has dramatically increased stability and uniform Zn deposition behavior. Remarkably, it exhibits a Coulombic efficiency of approximately 99.4 %, a long lifespan of around 3000 hours at the current density of 1 mA cm⁻² with a capacity of 0.5 mAh cm⁻². The excellent reversibility of zinc persists with current densities of 2, 5, and 10 mA cm⁻². Furthermore, Zn‐MnO₂ battery constructed with ZSi@Zn also delivers excellent performance, manifesting a capacity retention of 88.4 % after 4000 cycles.