Synergistic Modulation at Atomically Dispersed Fe/Au Interface for Selective CO2 Electroreduction.

The electrocatalytic carbon dioxide reduction reaction (CO2RR) offers an attractive route to fuels and feedstocks from renewable energy. Gold is active for the electrochemical CO2RR to CO, while the competing hydrogen evolution reaction is unavoidable. Here, we report a synergistic strategy, via introducing atomically dispersed Fe to tune the electronic structure of the Au nanoparticle, to improve the CO selectivity. By using operando X-ray absorption and infrared spectroscopies, we reveal the dynamic structural evolution and the adsorption of reactant intermediates at the single-atom Fe1/Au interface. During the reaction, the interaction between Fe and Au atoms becomes stronger, and the Fe1/Au synergies affect the adsorption of reaction intermediates, thus improving the selectivity of CO up to 96.3% with a mass activity of 399 mA mg-1. These results highlight the significant importance of synergistic modulation for advancing the single-atom decorated nanoparticle catalysis.