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 MoS₂ 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 MoS₂ 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.

通过调节合成水热温度，可控制地合成了一系列孔径和介孔结构可调的NiMo / FDU-12催化剂，并将其用于二苯并噻吩及其衍生物的加氢脱硫。最新的电子断层扫描显示，随着水热温度的升高，FDU-12载体的孔径增大，介孔结构从有序的笼型孔转变为局部无序的通道。同时，MoS ₂形态从小直条到半弯曲弧形再到球形，最后随着支撑结构的变化而变大。其中，在150℃水热处理的FDU-12具有合适的孔径和连通的孔结构，有利于高活性MoS ₂的形成。具有弯曲的形态 因此，其相应的催化剂表现出最好的HDS活性。此外，表明添加铝后，对于4，6-二甲基二苯并噻吩的HDS，异构化途径可以得到显着改善，这有望用于去除大分子硫化合物。我们的研究阐明了载体效应，活性位点形态与HDS性能之间的关系，并为开发高活性HDS催化剂提供了指导。