Citation: Wen-Wu ZHOU, Shi-Yu HAN, Zhi-Ping CHEN, Ying-Feng DUAN, Jie KANG, Fei FAN, Chang TIAN, Xin-Meng ZHANG. Hierarchical TS-1 zeolite loaded with NiMo catalysts: Preparation and performance in hydrodesulfurization[J]. Chinese Journal of Inorganic Chemistry, ;2023, 39(5): 891-905. doi: 10.11862/CJIC.2023.049 shu

Hierarchical TS-1 zeolite loaded with NiMo catalysts: Preparation and performance in hydrodesulfurization

Wen-Wu ZHOU ^{1, 2} ,
Shi-Yu HAN ¹ ,
Zhi-Ping CHEN ^{1, 2,,} ,
Ying-Feng DUAN ^{1, 2} ,
Jie KANG ¹ ,
Fei FAN ¹ ,
Chang TIAN ¹ ,
Xin-Meng ZHANG ¹

1.
College of Chemistry and Chemical Engineering, Xi′an University of Science and Technology, Xi′an 710054, China
2.
State Key Laboratory of Green and Safe Coal Development in Western China, Xi′an 710054, China

Corresponding author: Zhi-Ping CHEN, cupczp@163.com
Received Date: 5 December 2022
Revised Date: 23 March 2023

Figures(9)

The sole micropores strictly restrict the wide utilization of TS-1 zeolite in the catalytic fields, especially in the catalytic conversion of compounds with large molecular sizes. Here, we report a feasible and economical method to overcome this drawback. In this work, the hierarchical TS-1 zeolite was constructed via post-acid treatment, postalkali etching, and a combination of postacid treatment and alkali etching methods, after which, the corresponding NiMo-supported catalysts were prepared via the incipient wetness impregnation method. Then, the aforementioned materials were fully characterized using X - ray diffraction (XRD), N₂ adsorption - desorption, pyridine adsorbed Fourier transform infrared spectroscopy (Py - FTIR), H₂ temperature programmed reduction (H₂ - TPR), X-ray photoelectron spectroscopy (XPS), and high-resolution transition electron microscope (HR-TEM) to unravel the changes in the physicochemical properties caused by the post treatments. Finally, the hydrodesulfurization of dibenzothiophene (DBT) was used as a probe to assess the effects of the post-treatments on the catalytic performance of the hierarchical NiMo/TS-1 catalysts. The results showed that the MFI topology of TS-1 zeolite remained undamaged significantly and the serial hierarchical TS-1 zeolites exhibited higher specific surface areas and mesopore structures. Moreover, appropriate amounts of Br?nsted acid sites were formed at the surface of the serial hierarchical TS-1 zeolites. The interaction between the active metals and the support materials was also modulated by the posttreatment of TS-1 zeolite, which resulted in better dispersion of Ni promoted MoS₂ slabs with a higher proportion of NiMoS active phase, further leading to the enhanced catalytic activity and direct desulfurization pathway selectivity of the corresponding serial hierarchical NiMo/TS-1 catalysts. Among all the prepared catalysts, the catalytic activity was enhanced by approximately 1.2 times over catalyst NiMo/AT-TS-1 obtained by post-acid treatment compared to that over catalyst NiMo/TS-1 without treatment and on which the selectivity of the DDS pathway was 22% higher compared to that over catalyst NiMo/TS-1.
- hierarchical TS-1 zeolite,
- TS-1 zeolite loaded with NiMo catalyst,
- active phase,
- dibenzothiophene,
- hydrodesulfurization
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沈阳化工大学材料科学与工程学院沈阳 110142