Electrocatalytic CO2 coupling with nitrate to synthesize acetamide provides a promising way for the co-valorization of greenhouse gas and environmental pollutants. Aiming at generating acetamide via C─C─N bonding, a N-coordinated copper-cobalt diatomic catalytic sites is constructed to achieve CO2 reduction to ketene intermediate and NO3 - to ammonia, thereby facilitating the nucleophilic attack of *NH2 on *CH2CO to form acetamide. Based on the enhanced mass transfer of CO2 in flow cell, an acetamide yield of 67.7 mg L-1 and a FE of 15.1% are achieved over CuCo diatomic sites. In situ FT-IR, Raman spectroscopy, in situ XAFS combined with DFT suggest that CuCo diatomic pairs induce CO2 and NO3 - to stabilize on the catalytic surface via a favorable bridge adsorption configuration. And the electronic structure optimization promoted by interatomic electron interactions reduces the energy barriers for C─C and C─N bonding. This work achieves C─C─N bonding with ordered C─C and C─N coupling via diatomic sites, providing a novel strategy for the sustainable synthesis of acetamide.
Xu et al. (Tue,) studied this question.