期刊
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卷 151, 期 1, 页码 -出版社
SPRINGER
DOI: 10.1007/s10562-020-03290-0
关键词
Hydrodesulfurization (HDS); 4,6 Dimethyl-dibenzothiophene (4,6-DMDBT); Quinoline; Poisoning; Reaction pathway; Common intermediate mechanism
资金
- key project of Liaoning Province Natural Science Fund Project [20170540459]
- 47th batch Scientific Research Foundation for the Returned Overseas Chinese Scholars, State Education Ministry of China
- open objects of the major science and technology platform, Liaoning University of Science and Technology [USTLKFZD 201632]
The study found that the presence of quinoline and steric hindrance of methyl can alter the hydrodesulfurization pathway and exacerbate the transformation process. Quinoline has a relatively mild poisoning effect on DBT HDS, but when adjacent methyl is present, the inhibition on 4,6-DMDBT HDS is still significant. Additionally, quinoline affects the ratio of HYD/DDS pathway yield, increasing the production of HYD products.
Steric hindrance of methyl on reaction pathway of hydrodesulfurization in presence of quinoline was investigated over a NiMo/Al(2)O(3)catalyst at 4.0 MPa and 320 degrees C. The results show that steric hindrance of methyl changed the main pathway of HDS while presence of quinoline further exacerbated this transformation. Changes in inhibitory factor curve show that quinoline poisoning on DBT HDS is a relatively mild. When adjacent methyl is present, even at low concentration, the inhibitory factor of quinoline on 4,6-DMDBT HDS is still greater than 85%. At high levels, the inhibitory factor of quinoline on DDS pathway even exceeds 99%. Quinoline poisons HYD pathway of DBT HDS to a stable level in a short time (30 to 60 min). However, after 6 h of reaction, HYD pathway yield of 4,6-DMDBT HDS is still increasing. Quinoline simultaneously poisons HYD and DDS pathways of 4,6-DMDBT HDS to a stable level within 120 min, and then DDS pathway will continue to be poisoned, thereby increasing HYD pathway yield. Regardless of presence of adjacent methyl in sulfur-containing molecules, an increase in quinoline concentration will lead to an increase in HYD/DDS pathway yield ratio. Addition of quinoline inhibits conversion of hydrogenated intermediates to DDS products by poisoning C-S bond dissociation center (such as CUS active site) and leads to formation of deep hydrogenated products. Graphic
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