Ultra-selective desulfurization of 4, 6-dimethyldibenzothiophene via carbon-sulfur bond cleavage with the bimetal single atom on N-rGO

A single-atom Cu and Ni anchored on N-doped Reduced Graphene Oxides, which confer the intensified exposure of interior active sites, was developed. Due to single-atom active sites which accelerated the oxygenation and hydrogenation, the prepared Cu/Ni-N-rGO shows excellent conversion, good stability and selectivity for C-S bond cleavage by catalytic oxidation and hydrogenation at the different temperatures. The desulfurization ratio and selectivity for 4, 6-DMDBT to carbonhydrogen were 100 % and 100 %, respectively, on the suitable conditions. The kinetics of catalytic oxidation and in situ hydrogenation of 4, 6-DMDBT, and their mechanism over Cu/Ni-N-rGO by density functional theory was explored. Computational studies show the C-S cleavage of the 4, 6-dimethyldibenzothiophene by catalytic oxidation and then in situ hydrogenation is easier than that by direct hydrogenation or catalytic oxidation.