Catalytic hydrodeoxygenation of coal tar is a necessary process to upgrade its quality, improve its thermal stability, and reduce its corrosion. The design and preparation of catalyst is very important in the whole process. Based on our previous calculation research about the dibenzofuran hydrodeoxygenation on the Pt(111) and Ni(111) surfaces, the Ni-TiOx/SBA-15 catalyst is designed and prepared. The influence of the modification of Ni by TiO2 on dibenzofuran hydrodeoxygenation is revealed. The ring-opening and dehydroxylation reactions of six oxygen-containing intermediates on the Ni(111) surface and the interface sites between Ni nanoparticles and TiOx are firstly compared by density functional theory calculations. The results show that the unsaturated Ti3+ atom on Ti3O6 cluster and Ni atoms can co-adsorb the oxygen-containing intermediates at the interfacial site of Ni-TiOx/SBA-15 catalyst. This promotes the adsorption of oxygen-containing intermediates and activates C−O bonds, which reduces the ring-opening and dehydroxylation activation energies of these intermediates. The experimental results show that the modification of Ni metal by TiO2 can also inhibit cyclohexylphenoxy hydrogenation to cyclohexylphenol, thus promoting the formation of pentahydrocyclohexylphenol and improving the deoxidation reaction rate. Moreover, the addition of TiO2 improves the dispersion of Ni. This study may provide a new strategy for designing new catalysts for hydrodeoxygenation of oxygen-containing compounds in coal-based crude oil.

Dibenzofuran hydrodeoxygenation on Ni catalysts by surface decoration of TiO2-x species

ACS Spring Meeting 2021

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