Zincophilic Cu Sites Induce Dendrite‐Free Zn Anodes for Robust Alkaline/Neutral Aqueous Batteries

Metallic zinc (Zn) for next‐generation aqueous batteries often suffers from severe dendrite growth, unfavorable hydrogen evolution, and self‐corrosion, especially in alkaline electrolyte. Herein, the authors demonstrate a facile and efficient strategy to tackle above issues by electrochemically depositing Zn onto the Cu–Zn alloy surface (CZ‐Zn). The zincophilic Cu sites throughout the Cu–Zn alloy can remarkably enhance the Zn2+ adsorption and promote homogeneous Zn nucleation on its surface, endowing it with highly reversible Zn plating/stripping chemistry. Furthermore, the intrinsically inert nature of Cu toward hydrogen evolution reaction (HER) and high dezincification potential of the Cu‐Zn alloy can effectively alleviate the hydrogen evolution and Zn corrosion in aqueous electrolyte. Consequently, the symmetric cells with the CZ‐Zn electrodes exhibit outstanding cycling life in both alkaline and neutral electrolytes, which can operate steadily over 800 h and 1600 h at 2.5 mAh cm–2, respectively, far surpassing the pristine Zn electrodes. In addition, a high‐performance alkaline full battery with ultra‐long cyclic stability (no capacity degradation after 5000 cycles) and excellent Coulombic efficiency (CE) (100%) is achieved by pairing this CZ‐Zn anode with a Ni3S2@polyaniline cathode. This study sheds light on the design of robust and ultra‐stable Zn anodes for the state‐of‐art aqueous energy storage devices. An efficient strategy of introducing zincophilic Cu sites is demonstrated to induce dendrite‐free Zn anodes for the alkaline/neutral aqueous batteries. The strong zincophilicity and inert nature of Cu for hydrogen evolution reaction (HER) as well as high dezincification potential of Cu–Zn alloy facilitate homogeneous Zn nucleation, alleviate the hydrogen evolution and Zn corrosion, thus achieving an ultra‐stable Zn anode. The as‐fabricated symmetric cells with the CZ‐Zn electrodes exhibit outstanding cycling life in both alkaline and neutral electrolytes, which can operate steadily over 800 and 1600 h at 2.5 mAh cm−2, respectively, far surpassing the pristine Zn electrodes.