The microenvironments including the surface hydroxyls, the oxygen vacancies, and the d-band center of hierarchical TS-1 zeolite pickled by hydrochloric acid were regulated by ZrO2, the effect of ZrO2 on the physicochemical properties and the catalytic performances of the corresponding NiMoS supported catalysts were studied. The experimental and theoretical calculation results show that the d-band center, the surface hydroxyl groups, and the oxygen vacancies were regulated after incorporation of ZrO2. Resulting in the modulated acidity of the support and the metal support interaction of the catalysts, further promoting the formation of type-II NiMoS active phases. The catalytic performance evaluations show that catalyst NiMo/1-ZAT exhibits the superior HDS performance, kinetic study further demonstrated that the enhanced catalytic activity was mainly contributed by the improved direct desulfurization activity generated from the moderate support acidity, suitable MSI, highest sulfidation degrees, most type-II NiMoS active phase and highest activity of individual active sites.
