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.