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

Abstract

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.

Keywords: Janus nanostructures; asymmetric growth; carbon dioxide reduction reaction; facets; tandem catalysis.