郭新闻

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教授

博士生导师

硕士生导师

主要任职:盘锦校区管委会副主任兼教学与科研工作部部长

性别:男

毕业院校:大连理工大学

学位:博士

所在单位:化工学院

学科:工业催化. 物理化学

办公地点:化工实验楼B427

联系方式:18641143913

电子邮箱:guoxw@dlut.edu.cn

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Investigation of methanol conversion over high-Si beta zeolites and the reaction mechanism of their high propene selectivity

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论文类型:期刊论文

发表时间:2017-12-21

发表刊物:CATALYSIS SCIENCE & TECHNOLOGY

收录刊物:SCIE、EI

卷号:7

期号:4

页面范围:5882-5892

ISSN号:2044-4753

摘要:Large pore high-Si beta zeolites (Si/Al = 136 to 340) were synthesized by a HF-assisted method, and their catalytic performance for the conversion of methanol to propene was explored. It is demonstrated that beta zeolites with low acid density facilitate the achievement of high propene selectivity and a high propene/ethene ratio. The HF dosage in the synthesis has great influence on the Al distribution in the framework, as evidenced by Al-27 MAS NMR and Al-27 MQ MAS NMR spectroscopy, which may influence the acidity and microstructure of acid sites and lead to a remarkable catalytic lifespan. A HF/SiO2 ratio of 0.45 is found to facilitate the synthesis of high-Si beta enriched with Al atoms located at the T9 sites; this helps the catalyst show the longest lifetime, with a propene selectivity of 49.7-58.3% at 550 degrees C and WHSV = 2 h(-1). With the aid of C-12/C-13-methanol switch experiments, we elucidated that the olefin-based mechanism dominates the reaction and contributes to the formation of ethene, propene, and higher olefins. Moreover, two phenol compounds are identified in the coke species, which have not been observed previously and have been found to be detrimental to the reaction.