Design of promising single Rh atom catalyst for CO oxidation based on Graphdiyne sheets

Abstract Single-atom catalyst (SAC) have received increasing attention in the field of CO oxidation due to their higher catalytic activity and greater atomic utilization. The CO oxidation by O2 on the single Rh atom embeddedover Graphdiyne (Rh-GDY) is systematically studied by using the first principles simulation. It is found that Rh atom can be stably and isolated in the GDY as a single metal atom binding to the carbon atoms. Both of the Langmuir–Hinshelwood (LH) and the Trimolecular Eley-Rideal (TER) mechanisms are preferable due to the rather low reaction barrier of their rate-determining steps. Moreover, LH mechanism could be more preferable than the TER mechanism according to their reaction rate constants at various temperatures, indicating that Rh-GDY is a promising catalyst for CO oxidation. Our investigation would help to reveal the mechanisms of the CO oxidation on SAC and shed light on the design of SAC based on GDY sheets for the oxidation of the fuel gas.