Chelate‐Capped Nano‐AgZn₃ Dual Interphase Remodeling the Local Environment for Reversible Dendrite‐Free Zinc Anode

Abstract Rechargeable aqueous zinc‐ion batteries (AZIBs) are among the most promising candidates for next‐generation energy‐storage devices. However, the large voltage polarisation and infamous dendrite growth hinder the practical application of AZIBs owing to their complex interfacial electrochemical environment. In this study, a hydrophobic zinc chelate‐capped nano‐silver (HZC‐Ag) dual interphase is fabricated on the zinc anode surface using an emulsion‐replacement strategy. The multifunctional HZC‐Ag layer remodels the local electrochemical environment by facilitating the pre‐enrichment and de‐solvation of zinc ions and inducing homogeneous zinc nucleation, thus resulting in reversible dendrite‐free zinc anodes. The zinc deposition mechanism on the HZC‐Ag interphase is elucidated by density functional theory (DFT) calculations, dual‐field simulations, and in situ synchrotron X‐ray radiation imaging. The HZC‐Ag@Zn anode exhibited superior dendrite‐free zinc stripping/plating performance and an excellent lifespan of >2000 h with ultra‐low polarisation of ≈17 mV at 0.5 mA cm⁻². Full cells coupled with a MnO₂ cathode showed significant self‐discharge inhibition, excellent rate performance, and improved cycling stability for >1000 cycles. Therefore, this multifunctional dual interphase may contribute to the design and development of dendrite‐free anodes for high‐performance aqueous metal‐based batteries.