The CO oxidation on Mn atom embedded in N vacancy of C3N monolayer: A DFT-D study

Abstract

In this study, the use of a single Mn atom anchored to a nitrogen vacancy in a C3N monolayer ([email protected]3N) for CO oxidation is investigated using first-principles calculations. The stability of [email protected]3N is confirmed through the analysis of binding energy, the movement of the Mn atom within the N vacancy, and ab initio molecular dynamics simulations at 400K for a period of 6 ps. O2 is found to have more favorable adsorption on [email protected]3N compared to CO, and the direct dissociation barrier for O2 is only 0.69 eV. The Eley-Rideal (ER) and Langmuir-Hinshelwood (LH) mechanisms are also examined on the [email protected]3N, and it is found that the ER mechanism was preferred due to its lower rate limiting barrier (0.57 eV compared to 0.91 eV for the LH mechanism). In addition, the oxidation of CO by the leftover O atom on the [email protected]3N is found to be facile, with a small barrier of 0.05 eV via the ER mechanism. These findings provide insight into the potential of the [email protected]3N as a single-atom catalyst for CO oxidation at low temperatures.