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Gallium Modified HUSY Zeolite as an Effective Co‐support for NiMo Hydrodesulfurization Catalyst and the Catalyst's High Isomerization Selectivity
Author(s) -
Zhou Wenwu,
Zhou Yasong,
Wei Qiang,
Du Lin,
Ding Sijia,
Jiang Shujiao,
Zhang Yanan,
Zhang Qing
Publication year - 2017
Publication title -
chemistry – a european journal
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.687
H-Index - 242
eISSN - 1521-3765
pISSN - 0947-6539
DOI - 10.1002/chem.201701307
Subject(s) - isomerization , catalysis , hydrodesulfurization , zeolite , chemistry , selectivity , space velocity , inorganic chemistry , nuclear chemistry , organic chemistry
The effects of metal‐modified acidic co‐supports on the hydrodesulfurization (HDS) activity and isomerization selectivity of highly refractory organosulfur compounds such as 4,6‐dimethyldibenzothiophene have been investigated. Y zeolite crystals with high Si/Al ratios and small crystallite sizes were successfully synthesized by a new hydrothermal synthesis approach. The synthesized Y zeolite crystals were ion‐exchanged and stabilized. The prepared samples were then modified with different gallium contents using an impregnation method to adjust their acidity properties, and these modified samples were used as co‐supports for NiMo sulfide HDS catalysts. The catalyst containing 10 wt.% zeolite Y modified by 2 wt.% gallium (NiMo/2GaY‐ASA‐A) exhibited the highest HDS activity, with 4,6‐dimethyldibenzothiophene (4,6‐DMDBT) conversion nearly double the rate of the catalyst without zeolite at 563 K, 4.0 MPa and liquid hourly space velocity (LHSV) of 40 h −1 . NiMo/2GaY‐ASA‐A also exhibited superior isomerization ability, with 3,4′‐DMBP, 4,4′DMBP, and 3,6‐DMDBT as the main products, indicating that the isomerization pathway was the main reaction route over NiMo/2GaY‐ASA‐A. The superior catalytic performance is related to the synergistic effect of the proper amount of medium and strong Brønsted acid sites. The compounds 3,6‐DMDBT and 3,7‐DMDBT (isomers of 4,6‐DMDBT) and 3,4,6‐TMDBT and tetra‐methyl‐DBT (transmethyl products) were detected simultaneously in the HDS product of 4,6‐DMDBT for the first time over NiMo/GaY‐ASA‐A catalysts. Finally, a new reaction network over NiMo/2GaY‐ASA‐A was proposed.