Janus

Catalysis

Engineering

Electrochemistry

Metallurgy

Materials science

Density functional theory

Carbon monoxide

Inorganic chemistry

Chemical engineering

Electrocatalyst

Physical chemistry

Tandem

Nanotechnology

Organic chemistry

Computational chemistry

Composite material

Chemistry

Selectivity

Electrode

Nanostructure

Electrochemical reduction of carbon dioxide

Carbon dioxide

Copper

Advanced Materials

Electrocatalytic carbon dioxide reduction reaction (CO2 RR) holds significant potential to promote carbon neutrality. However, the selectivity toward multicarbon products in CO2 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 CO2 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, Ag65 -Cu35 JNS-100 demonstrates much superior selectivity for both ethylene and multicarbon products in CO2 RR at less negative potentials. Density functional theory calculations reveal that the compensating electronic structure and carbon monoxide spillover in Ag65 -Cu35 JNS-100 contribute to the enhanced CO2 RR performance. This study provides an effective strategy to design advanced tandem catalysts toward the extensive application of CO2 RR.

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