期刊
JOURNAL OF MATERIALS CHEMISTRY A
卷 2, 期 46, 页码 19738-19749出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c4ta03691c
关键词
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资金
- National NSFC [21276277]
- Opening Project of the Guangxi Key Laboratory of Petrochemical Source Processing and Process Intensification Technology [2012K01]
- CNPC-Petrochemical Research Key project
- PetroChina Innovation Foundation [2011D-5006-0403]
Mesoporous FDU-12 silicas with different morphologies have been synthesized under static and stirring conditions in a water bath. Furthermore, a series of mesoporous FDU-12 silicas modified by different amounts of titania have been synthesized, through a two-step method of prehydrolysis of TEOS followed by addition of titanium butoxide as a titanium precursor. Their respective NiMo supported catalysts were also prepared and characterized to elucidate the effects of titania, on the characteristics of the Mo surface species and their hydrodesulfurization (HDS) activities on dibenzothiophene (DBT) and 4,6-dimethyldibenzothiophene (4,6-DMDBT). The composites were characterized by various techniques (XRD, SEM, TEM, FT-IR, UV-vis, Si-29 NMR, Raman, XPS and N-2 adsorption-desorption); meanwhile, the catalysts were also tested in a higher pressure HDS reactor at T=340 degrees C and P=4 MPa with different liquid hourly space velocity (LHSV) values. The results show that the two-step synthetic route can prepare well-ordered mesoporous composites with high surface areas and large pore sizes and volumes. Obvious differences in the Mo species can be observed on the sulfided NiMo/Ti-FDU-12 catalysts. This showed that appropriate Ti loading could facilitate the dispersion of molybdena and the formation of the MoS2 and NiMoS phases, which are the important factors for the HDS reaction. All of the catalysts presented high HDS activity, and when the Si : Ti molar ratio was increased to 5, the HDS activities on DBT and 4,6-DMDBT could reach as high as 97% and 65% respectively.
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