CoMo series catalysts based on ZSM-22/PHTS (ZP) composite materials with different SiO2/Al2O3 molar ratios were prepared via the impregnation method. The properties of the ZP material and the corresponding catalysts were analyzed by a series of characterization methods. The hydro-upgrading performance of the catalysts was evaluated on a fixed-bed reactor under the operation conditions of 270 °C, 200 ml ml−1, 2.0 h−1, and 2.0 MPa. The catalyst with the ZP material as the support additive exhibited better activities than the reference CoMo-based Al2O3 and ZSM-22 catalysts. The CoMo/ZPA120 catalyst presented a good balance between hydrodesulfurization (HDS) activity (95.2%) and lower loss of research octane number (ΔRON = −1.1). The results suggested that the molybdenum–support interaction, the dispersion, and stacking states of MoS2 slabs were the key factors in forming sufficient type II CoMoS active phases for better catalytic activity.
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