Endogenous Organic–Inorganic Hybrid Interface for Reversible Zn Electrochemistry

Abstract Despite rechargeable aqueous Zn‐ion batteries (AZIBs) exhibit advantages such as high safety, high specific energy, and low cost, etc, the implementation of Zn anodes is still hampered by insufficient cyclability and grievous side reactions. To improve the cycling stability of the zinc anode, a stable zinc anode/electrolyte interface is needed to suppress dendrite formation and side reactions. Herein, a self‐regulating endogenous organic–inorganic hybrid interface layer (EHI) in situ on the surface of the Zn anode by regulating solvent molecules is constructed. The EHI consists of an organic outer layer containing N─H and ─CH₃ and an inorganic inner layer containing ZnO and ZnCO₃, which effectively inhibits hydrogen evolution and dendrite growth. Consequently, AZIBs with the EHI achieve a lifespan exceeding 5500 h in 3 mA cm⁻², and stripping/plating on copper foils for 600 cycles with an average coulomb efficiency (CE) of 99.47%. This study provides a feasible idea for realizing stable and reversible zinc‐ion batteries.