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.