Enhanced Catalytic Oxidation of CO on Sulfur-Doped Boron Nitride

Bridging the gap between homogeneous and heterogeneous catalysis, the single-atom catalyst supported on a substrate shows extremely high atom efficiency, low cost, excellent stability, and high activity for CO oxidation. Here, we report the catalytic mechanism of CO oxidation on sulfur-doped h-BN. The chemisorption activates O-2 via electron transfer from sulfur-doped h-BN, inducing a reduction in the bond order of O-2 and lengthening the O-O distance. This variation is helpful for the subsequent oxidation of CO. The oxidation process includes O-2 adsorption, electron reorganization, and two instances each of CO adsorption, oxygen transfer, and CO2 desorption. The first oxygen transfer from O-2 to CO occurs exothermically by similar to-63.8 kcal/mol with a barrier of similar to 12.1 kcal/mol, which is thus the rate-determining step. The significantly enhanced catalytic performance implies that sulfur doping on h-BN should have potential applications in the areas of metal-free catalysts with low cost and high activity.