methanol synthesis

electrochemical reduction

carbon nanotubes

catalytic activity

reduction reaction

faradaic efficiency

activity selectivity

synergistic effect

Advanced Materials

Electrocatalytic carbon dioxide reduction reaction (CO 2 RR) holds significant potential to promote carbon neutrality. However, the selectivity toward multicarbon products in CO 2 RR is still too low to meet practical applications. Here the authors report the delicate synthesis of three kinds of Ag–Cu Janus nanostructures with {100} facets (JNS‐100) for highly selective tandem electrocatalytic reduction of CO 2 to multicarbon products. By controlling the surfactant and reduction kinetics of Cu precursor, the confined growth of Cu with {100} facets on one of the six equal faces of Ag nanocubes is realized. Compared with Cu nanocubes, Ag 65 –Cu 35 JNS‐100 demonstrates much superior selectivity for both ethylene and multicarbon products in CO 2 RR at less negative potentials. Density functional theory calculations reveal that the compensating electronic structure and carbon monoxide spillover in Ag 65 –Cu 35 JNS‐100 contribute to the enhanced CO 2 RR performance. This study provides an effective strategy to design advanced tandem catalysts toward the extensive application of CO 2 RR.

Confined Growth of Silver–Copper Janus Nanostructures with {100} Facets for Highly Selective Tandem Electrocatalytic Carbon Dioxide Reduction