Cu-doped MoSi2N4 monolayer as a highly efficient catalyst for CO reduction toward C2+products

The electrochemical reduction of CO to valuable C2+ chemicals powered by renewable electricity provides a fascinating way to achieve carbon-neutral. However, the current catalysts generating C2+ products still face the challenge of ultra-high energy barrier for C-C bond formation and carbon-chains upgradation. Herein, a newly developed low dimensional material MoSi2N4 doped by one Cu atom (denoted as Cu-MSN) with three adjacent active N sites is proposed for CO reduction catalyst by means of the first-principles calculations. On the designed Cu-MSN catalyst, the adjacent active N sites nearby Cu atom are revealed to possess high efficiency for carbon chain upgradation with the almost negligible kinetic barrier of 0.04 eV. Particularly, CH4, C2H4, C2H6, C2H5OH and C3H7OH are identified as the main products with the free energy barriers lower than 0.57 eV. Our work not only provides a novel CO reduction catalyst, but also opens the way of MoSi2N4 in the area of CO reduction reaction.