Atomically Dispersed Ni/Cu Dual Sites for Boosting the CO 2 Reduction Reaction

Developing diatomic catalysts (DACs) for the CO 2 reduction reaction (CO 2 RR) has emerged as a promising leading-edge research area owing to their maximum atomic utility and more sophisticated functionalities. However, the proper design of DACs at an atomic level and an understanding of the synergistic mechanism of binary sites remain challenging. Herein, an N-rich carbon matrix with precisely controlled Ni/Cu dual sites is synthesized through the assistance of metal–organic frameworks. The as-prepared catalyst presents high CO Faradaic efficiency of over 95% from −0.39 to −1.09 V vs reversible hydrogen electrode (RHE) with the maximum value of 99.2% at −0.79 V vs RHE and long-term durability of 60 h electrolysis. Density functional theory studies reveal that the electronic redistribution and band gap narrowing induced by the adjacent NiN 4 and CuN 4 moieties enhance the electron conductivity and strengthen the bonding interactions between *COOH intermediates and Ni centers, thus lowering the overall reaction barriers and promoting CO generation.