A DFT study on the possibility of using a single Cu atom incorporated nitrogen‐doped graphene as a promising and highly active catalyst for oxidation of CO

Abstract

AbstractUsing dispersion‐corrected density functional theory (DFT) calculations, a single Cu adatom incorporated nitrogen‐doped graphene (CuN3‐Gr) is proposed as a new and highly active noble‐metal‐free catalyst for carbon monoxide (CO) oxidation reaction. According to our results, the Cu adatom can be stably anchored onto the monovavancy site of the nitrogen‐doped graphene, and the resulting large diffusion barrier suggests that the metal clustering is avoided in CuN3‐Gr. Three possible reaction mechanisms for CO oxidation (ie, Eley–Rideal, Langmuir–Hinshelwood, and termolecular Eley–Rideal) are systematically studied. It is found that the activation energy for the rate‐determining step of the termolecular Eley–Rideal mechanism is only 0.13 eV, which is much smaller than those of others. The results of this study may provide a useful guideline for the design of highly active and promising single‐metal catalysts for the CO oxidation reaction based on graphene.