A Robust Dual‐layer Interphase with Zincophilic and Anticorrosion Properties for Stabilizing Zn Metal Anodes

Abstract The construction of an artificial interphase for a stable metallic zinc (Zn) anode is an effective method to achieve excellent electrochemical performance for aqueous Zn metal batteries. In this report, a dual‐layer interphase of silver and titanium dioxide nanoparticles is rationally designed on the Zn electrode surface based on enhancing Zn affinity and interfacial anticorrosion, which enables multifunctional regulation of the electrode/electrolyte interface, improving electrochemical stability and uniform Zn deposition. Specifically, in this dual‐layer interphase architecture, the underlying zincophilic interphase can balance the interfacial electric field and achieve homogeneous initial Zn nucleation. The vacancy effect of the anticorrosion interphase at the upper layer regulates the Zn ion migration kinetics, thereby inducing dendrite‐free Zn deposition behavior. As a result, the advanced Zn symmetric cells deliver an excellent cycling performance (3800 h at 1.0 mA cm ⁻² /1.0 mAh cm ⁻² and 2000 h at 5.0 mA cm ⁻² /2.0 mAh cm ⁻² ), and the assembled AT@Zn//I ₂ cell achieves stable operation of 5000 cycles at 2.0 C. This concept of a dual‐layer interphase design presents an appealing avenue for reversible Zn metal anodes.