Potential of transition metal atoms embedded in buckled monolayer g-C3N4 as single-atom catalysts

Abstract

We use first-principles calculations to systematically explore the potential of transition metal atoms (Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Ru, Rh, Pd, Ag, Ir, Pt, and Au) embedded in buckled monolayer g-C₃N₄ as single-atom catalysts. We show that clustering of Sc and Ti on g-C₃N₄ is thermodynamically impeded and that V, Cr, Mn, and Cu are much less susceptible to clustering than the other TM atoms under investigation. Strong bonding of the transition metal atoms in the cavities of g-C₃N₄ and high diffusion barriers together are responsible for single-atom fixation. Analysis of the CO oxidation process indicates that embedding of Cr and Mn in g-C₃N₄ gives rise to promising single-atom catalysts at low temperature.