Structural Design and Interface Modification with Selective H⁺ Binding of 3D Zinc Anode for Aqueous Zinc‐Ion Batteries

Abstract The reversible cycling lifespan of zinc‐ion batteries is fundamentally compromised by the hydrogen evolution reaction (HER) and the growth of Zn dendrites induced by tips on 2D zinc metal anodes. Herein, a 3D zinc metal alloy anode to effectively mitigate dendrite growth and HER through dual regulation of the interface is presented. Experimental results confirm that the second component with strong H⁺ adsorption can efficiently inhibit H_ads desorption diffusion, thereby suppressing HER. Moreover, the robust interaction between the in‐situ derived solid electrolyte interphase (SEI) layer and Zn²⁺ also enhances Zn²⁺ diffusion kinetics, reduces nucleation energy barriers, achieving dendrite‐free deposition of Zn²⁺. The as‐prepared 3D Zn‐W anodes achieve a lifespan of up to 2400 h with a coulombic efficiency of 99.23% achieved in symmetrical cells and can also exceed 200 h when operated at a depth of discharge as high as 91.46%. This work provides a simple and effective approach toward enhancing the safety and efficiency of zinc‐ion batteries while significantly improving Zn utilization efficiency.