Protective mass-charge transfer regulation layer via magnetron co-sputtering towards stable Zn anodes

The practical implementation of zinc (Zn) metal anodes in large-scale aqueous energy storage systems is severely hindered by interfacial instabilities, including dendritic Zn growth, parasitic hydrogen evolution, and self-corrosion. Here, we report a mechanism-driven interfacial design strategy guided by the mass–charge transfer equilibrium within the electric double layer, which dictates the Zn nucleation and growth behavior. Based on this insight, we construct a corrosion-resistant TaF_x (TF) interphase via magnetron co-sputtering, which mitigates ion depletion near the Zn surface and promotes spatially uniform Zn electrodeposition. Concurrently, the TF layer elevates the energy barrier for hydrogen evolution and imparts robust corrosion resistance, thereby suppressing interfacial side reactions. These synergistic effects collectively enable planar, dendrite-free Zn deposition and stripping over 1000 cycles with a high Coulombic efficiency of 99.87 %. When integrated into a full-cell configuration with a NH₄V₄O₁₀ cathode, the TF-modified Zn anode retains 82.5 % of its initial capacity after 250 cycles at a current density of 0.5 A g^-1. This work establishes a mechanistic framework for interfacial engineering of Zn metal anodes and offers a broadly applicable strategy for stabilizing high-performance AZIBs.