A Comparative Study of CO Oxidation on Nitrogen‐ and Phosphorus‐Doped Graphene

The geometry, electronic structure, and catalytic properties of nitrogen‐ and phosphorus‐doped graphene (N‐/P‐graphene) are investigated by density functional theory calculations. The reaction between adsorbed O 2 and CO molecules on N‐ and P‐graphene is comparably studied via Langmuir–Hinshelwood (LH) and Eley–Rideal (ER) mechanisms. The results indicate that a two‐step process can occur, namely, CO+O 2 →CO 2 +O ads and CO+O ads →CO 2 . The calculated energy barriers of the first step are 15.8 and 12.4 kcal mol −1 for N‐ and P‐graphene, respectively. The second step of the oxidation reaction on N‐graphene proceeds with an energy barrier of about 4 kcal mol −1 . It is noteworthy that this reaction step was not observed on P‐graphene because of the strong binding of O ads species on the P atoms. Thus, it can be concluded that low‐cost N‐graphene can be used as a promising green catalyst for low‐temperature CO oxidation.