Tuning low-temperature CO oxidation activities via N-doping on graphene-supported three-coordinated nickle...

Nitrogen doping is identified as an intriguing way to regulate graphene-supported single-atom catalysts (SACs) for heterogeneous catalysis. However, little theoretical effort has been directed towards exploring the activity trend in terms of N-doping level. In this study, we systematically investigated the N-doping effect on CO oxidation activities for graphene-supported three-coordinated Ni SACs (Ni-NC_3-) in virtue of density functional theory (DFT) calculations and microkinetic modeling. We found that N-doping will shift the d-band center of single-atom Ni upwards, enhance the adsorption of intermediates, and tune the activation barrier to the overall reaction activities. Ni-N₁C₂ exhibits excellent catalytic performance with the highest total reaction rate comparable to that of noble metal SACs. These findings are helpful for understanding the N-doping influence and rationalizing the art of designing novel SACs for CO oxidation at low temperatures.