UCLA

Next‐generation zinc (Zn)–based aqueous batteries are appealing for large‐scale energy storage due to their inherent safety and cost advantages, yet they often suffer from dendritic Zn growth, hydrogen evolution, and byproducts such as zinc hydroxides. Herein, we propose a gradient zincophilic anode fabricated via pulse electrodeposition of copper onto carbon paper, aiming to mitigate these challenges while enhancing Zn plating/stripping reversibility. In this approach, carefully controlled pulse plating deposits copper selectively across the porous carbon matrix, effectively lowering Zn nucleation and plating overpotentials by up to 40 % compared to bare carbon paper. During early galvanostatic cycling, the gradient‐coated electrodes reach nucleation potentials around 0.18–0.20 V (vs. Zn/Zn²⁺) and plating potentials near 0.20–0.21 V, whereas bare carbon typically remains above 0.28 V and climbs to 0.35 V or higher over repeated cycles. This improved zincophilicity translates into higher coulombic efficiencies (often 95–100 %) for the gradient coatings in the first 60–80 cycles. Although fully conformal Cu coatings also lower overpotentials and deliver 95–98 % efficiency, the gradient design can surpass conformal coverage in the early cycles. Longer‐term advantages of gradient Cu—such as deeper Zn infiltration or reduced dendrite formation—warrant further investigation, yet these findings underscore the crucial role of tailored copper modifications in overcoming Zn anode limitations and advancing practical aqueous zinc battery systems.