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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 CS 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 CS cleavage of the 4, 6-dimethyldibenzothiophene by catalytic oxidation and then in situ hydrogenation is easier than that by direct hydrogenation or catalytic oxidation.
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| http://dx.doi.org/10.1016/j.jhazmat.2020.122803 | DOI Listing |
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