Fe-doped C3N monolayer as a promising SAC for CO oxidation with low temperature and high reactivity

[Display omitted] •Structural and electronic behavior of Fe-embedded N-vacancy C3N monolayer is studied.•Fe-embedded C3N monolayer is determined as a novel SAC for CO oxidation.•CO and O2 adsorption on Fe-C3N monolayer are comprehensively analyzed. In this work, we investigate the CO oxidation on the Fe-doped N-vacancy C3N (Fe-C3N) monolayer by first-principle theory. Single Fe atom is doped on the N-vacancy site of C3N surface with a binding energy of −6.65 eV. The better performance of Fe-C3N upon O2 adsorption determines the preferred CO oxidation pathway by Eley-Rideal (ER) mechanism. Results indicate that the energy barriers in the two steps of ER mechanism are obtained as 0.45 and 0.47 eV, which could be feebly overcome at room temperature. Moreover, the physicochemical properties of the recovered Fe-C3N monolayer are unchanged compared with the original counterpart, manifesting that the CO oxidation on the Fe-C3N monolayer is energy-favorable at room temperature and the strong potential of Fe-C3N monolayer as a promising single-atom catalyst (SAC) for CO oxidation with high reactivity and low temperature. This work would be meaningful for the exploration of novel SAC in the field of heterogeneous catalysis.