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A series of NiMo/FDU-12 catalysts with tunable pore diameters and mesostructures have been controllably synthesized by adjusting the synthetic hydrothermal temperature and applied for the hydrodesulfurization of dibenzothiophene and its derivative. The state-of-the-art electron tomography revealed that the pore sizes of FDU-12 supports were enlarged with the increase in the hydrothermal temperature and the mesostructures were transformed from ordered cage-type pores to locally disordered channels. Meanwhile, the MoS 2 morphology altered from small straight bar to semibending arc to spherical shape and finally to larger straight bar with the change of support structures. Among them, FDU-12 hydrothermally treated at 150 °C possessed appropriate pore diameter and connected pore structure and was favorable for the formation of highly active MoS 2 with curved morphology; thus, its corresponding catalyst exhibited the best HDS activity. Furthermore, it was indicated that the isomerization pathway could be significantly improved for HDS of 4,6-dimethyldibenzothiophene after the addition of aluminum, which was expected to be applied to the removal of the macromolecular sulfur compounds. Our study sheds lights on the relationship between support effect, active sites morphology and HDS performance, and also provides a guidance for the development of highly active HDS catalysts.

The oxidation of TH to SP by H2O2 with the assistance of IL experiences two steps via two transition states.

FDU-12 silica with highly ordered face-centered cubic mesoporous structure is developed as support to prepare Mo/FDU-12 catalysts for hydrodesulfurization (HDS) of dibenzothiophene (DBT). A series of Mo/FDU-12 catalysts are synthesized by using incipient wetness impregnation method with different MoO3loadings (6, 8, 10, 12, and 15 wt.%). The objective of this work is to explore the pore confinement effect of FDU-12 mesochannels on the MoS2morphology with various metal loadings. It is found that, as increasing MoO3loadings from 6 to 15 wt.%, the MoS2nanocrystallites transform from monolayer to multilayer and the morphology changes from straight layered to curved and then to ring-like and finally to spherical-like morphology due to the restriction of cage-like pore channels of FDU-12 support. The HDS results show that the catalytic activity increases first and then decreases with the best HDS performance at the MoO3loading of 10 wt.%. In addition, we compared the HDS activity of Mo catalyst supported on FDU-12 with that on the commercialγ-Al2O3and SBA-15; the result exhibits that FDU-12 is superior to the other two supports due to its large pore size and ordered three-dimensional open pore channels.