Sabatier Principle Inspired Bifunctional Alloy Interface for Stable and High‐Depth Discharging Zinc Metal Anodes

Achieving stable Zn anodes is essential for advancing high‐performance Zn metal batteries. Here, we propose a Sabatier principle inspired bifunctional transition‐metal (TM) interface to enable homogeneous Zn dissolution during discharging and dendrite‐free Zn deposition during charging. Among various TM‐coated Zn (TM@Zn) electrodes, Cu@Zn exhibits the highest reversibility and structural stability, attributed to the optimal interaction between Cu and Zn. The heteroatomic interaction‐dependent electrochemical performance parallels the Sabatier principle. Morphological analyses reveal that bare Zn anodes display detrimental etching pits during stripping, which is different from the uniform dissolution for Cu@Zn electrodes. During subsequent plating, the conductive interface serves as a secondary current collector for uniform Zn deposition in Cu@Zn, thus demonstrating a bifunctional nature. Atomic observations disclose the working mechanisms of this interface as a gradual phase transition from Cu to CuZn5 during cycling. The Cu@Zn anodes exhibit an ultralong cycling lifespan of over 8000 h at a low current of 1 mA cm‐2 and over 250 h at a high depth of discharge of 80%. They also demonstrate practical feasibility by maintaining 88.7% capacity retention after 1000 cycles in Cu@Zn||VO2 full cells. This work provides new insights into the Sabatier chemistry inspired bifunctional layers for Zn metal battery system.