In Situ Construction of a Dual‐Component Hybrid Interfacial Layer for Stabilizing Zinc Anodes in Aqueous Zn‐Ion Batteries

Abstract Interfacial instability, particularly uncontrollable zinc deposition and water induced side reactions, severely compromises the cycling stability and lifespan of aqueous zinc‐ion batteries (AZIBs), thereby hindering their commercialization. Herein, an in situ grown bilayer gradient hydrophobic artificial interface (ZFPB) is designed to achieve dendrite‐free zinc deposition. In detail, the ion‐conductive but electronically insulating ZnF ₂ outer layer facilitates the rapid migration of Zn ²⁺ . Concurrently, the conductive Pb inner layer forms strong interactions with Zn ²⁺ through its valence electrons, effectively lowering the Zn ²⁺ adsorption energy and facilitating uniform Zn deposition. Moreover, the hydrophobic nature of ZFPB effectively suppresses interfacial water‐induced side reactions and mitigates anode corrosion. Benefiting from these synergistic advantages, the ZFPB//ZFPB symmetric cell exhibits a long cycle life of up to 2500 h at 5 mA cm ⁻² /1 mAh cm ⁻² . The ZFPB//MnO ₂ full cell retains 92.0% of its specific capacity after 2000 cycles. More encouragingly, it also delivers excellent electrochemical performance with a long cycling life of 700 cycles under a low N/P ratio of 1.8. This work offers valuable insights for the industrial advancement of AZIBs.