Zinc‐Contained Alloy as a Robustly Adhered Interfacial Lattice Locking Layer for Planar and Stable Zinc Electrodeposition

Abstract Stable zinc (Zn)/electrolyte interface is critical for developing rechargeable aqueous Zn‐metal batteries with long‐term stability, which requires the dense and stable Zn electrodeposition. Herein, an interfacial lattice locking (ILL) layer is constructed via the electro‐codeposition of Zn and Cu onto the Zn electrodes. The ILL layer shows a low lattice misfit (δ = 0.036) with Zn(002) plane and selectively locks the lattice orientation of Zn deposits, enabling the epitaxial growth of Zn deposits layer by layer. Benefiting from the unique orientation‐guiding and robustly adhered properties, the ILL layer enables the symmetric Zn||Zn cells to achieve an ultralong life span of >6000 h at 1 mA cm⁻² and 1 mAh cm⁻², a low overpotential (65 mV) at 10 mAh cm⁻², and a stable Zn plating/stripping for >90 h at an ultrahigh Zn depth of discharge (≈85%). Even with a limited Zn supply and a high current density (8.58 mA cm⁻²), the ILL@Zn||Ni‐doped MnO₂ cells can still survive for >2300 cycles.