The theoretical study of Rh single atom catalysts decorated C3N monolayer with N vacancy for CO oxidations.

In this work, the single Rh atom anchored by N vacancy of C3N monolayer for CO oxidations has been studied by using first-principles calculations. The stability for a single Rh atom in N vacancy of C3N monolayer is detailed investigated. The sizeable binding energy and diffusion barrier of the Rh atom in the N vacancy and the ab initial molecule dynamic simulations at 400 K all verify that the Rh is stable at the N vacancy of the C3N monolayer. We also have examined the bi-molecule Eley–Rideal (ER) and Langmuir–Hinshelwood (LH) and the tri-molecule LH mechanisms on the Rh @ C3N. It is found that the barriers for the rate-limiting step for bi-molecule ER and LH are so significant (1.35, 1.15 eV), while for the tri-molecule LH mechanism, the barrier of the rate-limiting step is only 0.49 eV, which means the tri-molecule LH mechanism is more likely to occur at room temperature on the Rh @ C3N. Thus, our results will shed light on the future design for low-temperature CO oxidation using single-atom catalysts. [ABSTRACT FROM AUTHOR]