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Three‐dimensional (3D) interconnected metal alloy nanostructures possess superior catalytic performance owing to their advantageous characteristics, including improved catalytic activity, corrosion resistance, and stability. Hierarchically structured Ni‐Cu alloys composed of 3D network‐like microscopic branches with nanoscopic dendritic feelers on each branch were crafted by a facile and efficient hydrogen evolution‐assisted electrodeposition approach. They were subsequently exploited for methanol electrooxidation in alkaline media. Among three hierarchically structured Ni‐Cu alloys with different Ni/Cu ratios (Ni0.25Cu0.75, Ni0.50Cu0.50, and Ni0.75Cu0.25), the Ni0.75Cu0.25 electrode exhibited the fastest electrochemical response and highest electrocatalytic activity toward methanol oxidation. The markedly enhanced performance of Ni0.75Cu0.25 eletrocatalyst can be attributed to its alloyed structure with the proper Ni/Cu ratio and a large number of active sites on the surface of hierarchical structures.  相似文献   
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