Dual-atom Ag2/graphene catalyst for efficient electroreduction of CO2 to CO

Abstract Electrochemical reduction of CO2 into value-added carbon compounds offers a promising strategy to mitigate global warming, but present challenges for chemistry due to the poor selectivity and stability of electrocatalysts. In this work, we report a dual-atom Ag2/graphene catalyst featuring well-defined AgN3-AgN3 active site for CO2 electrochemical reduction. This dual-atom catalyst can drive CO2 reduction reaction at a potential as high as -0.25 V, and exhibit excellent CO Faradic efficiency up to 93.4 % with a current density of 11.87 mA cm−2 at -0.7 V and long-term stability, far surpassing the single-atom Ag1/graphene and the traditional silver nanoparticle catalysts. DFT calculations reveal that the dual-atom Ag site lowers the barrier for the formation of *COOH by stabilizing the *CO2 through the concomitant interactions with the C and an O atom of CO2, resulting in excellent catalytic performance.