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

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.