Investigation of methanol conversion over high-Si beta zeolites and the reaction mechanism of their high propene selectivity
文献类型:期刊论文
作者 | Zhao, Xuebin1,2,3; Wang, Linying3; Li, Jinzhe3; Xu, Shutao3; Zhang, Wenna1,3; Wei, Yingxu3; Guo, Xinwen2; Tian, Peng3; Liu, Zhongmin3 |
刊名 | CATALYSIS SCIENCE & TECHNOLOGY |
出版日期 | 2017-12-21 |
卷号 | 7期号:4页码:5882-5892 |
ISSN号 | 2044-4753 |
DOI | 10.1039/c7cy01804e |
文献子类 | Article |
英文摘要 | 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. |
WOS关键词 | TO-OLEFIN CONVERSION ; CATALYZED METHYLATION REACTIONS ; UOP/HYDRO MTO PROCESS ; ANGLE-SPINNING NMR ; CO-REACTION ; HYDROCARBONS REACTION ; PRODUCT SELECTIVITY ; MOLECULAR-SIEVES ; H-BETA ; METHYLCYCLOPENTENYL CATIONS |
WOS研究方向 | Chemistry |
语种 | 英语 |
出版者 | ROYAL SOC CHEMISTRY |
WOS记录号 | WOS:000417712800009 |
源URL | [http://cas-ir.dicp.ac.cn/handle/321008/168418] |
专题 | 大连化学物理研究所_中国科学院大连化学物理研究所 |
通讯作者 | Tian, Peng; Liu, Zhongmin |
作者单位 | 1.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 2.Dalian Univ Technol, State Key Lab Fine Chem, PSU DUT Joint Ctr Energy Res, Sch Chem Engn, Dalian 116024, Peoples R China 3.Chinese Acad Sci, Natl Engn Lab Methanol Olefins, Dalian Natl Lab Clean Energy, Dalian Inst Chem Phys, Dalian 116023, Peoples R China |
推荐引用方式 GB/T 7714 | Zhao, Xuebin,Wang, Linying,Li, Jinzhe,et al. Investigation of methanol conversion over high-Si beta zeolites and the reaction mechanism of their high propene selectivity[J]. CATALYSIS SCIENCE & TECHNOLOGY,2017,7(4):5882-5892. |
APA | Zhao, Xuebin.,Wang, Linying.,Li, Jinzhe.,Xu, Shutao.,Zhang, Wenna.,...&Liu, Zhongmin.(2017).Investigation of methanol conversion over high-Si beta zeolites and the reaction mechanism of their high propene selectivity.CATALYSIS SCIENCE & TECHNOLOGY,7(4),5882-5892. |
MLA | Zhao, Xuebin,et al."Investigation of methanol conversion over high-Si beta zeolites and the reaction mechanism of their high propene selectivity".CATALYSIS SCIENCE & TECHNOLOGY 7.4(2017):5882-5892. |
入库方式: OAI收割
来源:大连化学物理研究所
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