Interface‐Engineered Zincophilic‐Zincophobic Bilayer Architecture for Stable Aqueous Zinc Metal Anodes

Abstract Aqueous zinc‐ion batteries (AZIBs) offer intrinsic safety and low cost, positioning them as promising candidates for large‐scale energy storage. However, uncontrolled Zn dendrite growth and parasitic hydrogen evolution reactions (HER) at the anode impede practical deployment. To address this, a dual‐interfacial layer (BN@Sn@Zn) combining zincophilic Sn and zincophobic boron nitride (BN) is engineered. This architecture regulates initial Zn ² ⁺ nucleation and subsequent deposition, suppressing dendrite formation while exploiting BN's high hydrogen adsorption energy to inhibit HER. The low ionic diffusion barrier of this bilayer synergistically enhances kinetics and enables rapid Zn ² ⁺ transport, facilitating homogeneous deposition. Consequently, the modified anode achieves a prolonged cycling lifespan of 1050 h at 6 mA cm ⁻² , 6 mAh cm ⁻² . In full‐cell configuration with MnO ₂ cathode, it retains 75 mAh g ⁻¹ after 2000 cycles, demonstrating superior stability versus bare Zn counterparts. This work innovates dual‐functional interfaces to optimize Zn deposition dynamics, advancing high‐performance AZIBs for sustainable energy storage systems.