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Influence of Support Acidity on the HDS Performance over β-SBA-16 and Al-SBA-16 Substrates: A Combined Experimental and Theoretical Study

Author:
Zheng, Peng, Hu, Di, Meng, Qian, Liu, Cong, Wang, Xilong, Fan, Jiyuan, Duan, Aijun, Xu, Chunming
Source:
Energy & fuels 2019 v.33 no.2 pp. 1479-1488
ISSN:
1520-5029
Subject:
Bronsted acids, Raman spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy, acidity, aluminum, aluminum oxide, catalysts, composite materials, density functional theory, fuels, nitrogen, nuclear magnetic resonance spectroscopy, pyridines, seeds, silicon, stable isotopes, transmission electron microscopy
Abstract:
A novel composite material β-SBA-16 is successfully synthesized and utilized as the support for the development of hydrodesulfurization (HDS) catalyst. The supports and the corresponding catalysts were characterized by a variety of techniques involving X-ray diffraction, N₂ physisorption, ²⁷Al NMR, Raman, pyridine IR, X-ray photoelectron spectra, and high-resolution transmission electron microscopy. The activity evaluation results displayed that the NiMo/β-SBA-16 catalyst possessed the highest dibenzothiophene HDS efficiency of 97.3% at weight hourly space velocity of 20 h–¹ compared with the catalysts supported on the Al-modified SBA-16 and the conventional Al₂O₃. Furthermore, the HDS efficiency of NiMo/β-SBA-16 is almost 1.5 times that of the other two catalysts at 150 h–¹, which was considered to be closely linked to the acidic properties of the supports. Correspondingly, the results of pyridine IR exhibited that NiMo/β-SBA-16 possessed larger amounts of total acidity and higher B/L acidities ratio. Furthermore, density functional theory calculations were performed to explore the Brønsted acid strength generated by the incorporation of β seeds or Al atoms. The calculation results indicated that Si atoms located in the 5- or 6-membered rings of β-zeolite were more easily substituted by Al atoms, and the generated Si–OH–Al group played an important role in providing stronger Brønsted acid sites. Therefore, both experimental and theoretical results have shown that the incorporation of β seeds contributed more to produce the Brønsted acid sites of SBA-16 materials.
Agid:
6313455