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Investigation of methanol conversion over high-Si beta zeolites and the reaction mechanism of their high propene selectivity
Zhao, Xuebin1,2,3; Wang, Linying1; Li, Jinzhe1; Xu, Shutao1; Zhang, Wenna1,2; Wei, Yingxu1; Guo, Xinwen3; Tian, Peng1; Liu, Zhongmin1
Source PublicationCATALYSIS SCIENCE & TECHNOLOGY
2017-12-21
ISSN2044-4753
DOI10.1039/c7cy01804e
Volume7Issue:4Pages:5882-5892
Indexed BySCI
SubtypeArticle
WOS HeadingsScience & Technology ; Physical Sciences
WOS SubjectChemistry, Physical
WOS Research AreaChemistry
WOS KeywordTO-OLEFIN CONVERSION ; CATALYZED METHYLATION REACTIONS ; UOP/HYDRO MTO PROCESS ; ANGLE-SPINNING NMR ; CO-REACTION ; HYDROCARBONS REACTION ; PRODUCT SELECTIVITY ; MOLECULAR-SIEVES ; H-BETA ; METHYLCYCLOPENTENYL CATIONS
AbstractLarge 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.
Language英语
WOS IDWOS:000417712800009
PublisherROYAL SOC CHEMISTRY
Citation statistics
Cited Times:10[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/168419
Collection中国科学院大连化学物理研究所
Corresponding AuthorTian, Peng; Liu, Zhongmin
Affiliation1.Chinese Acad Sci, Natl Engn Lab Methanol Olefins, Dalian Natl Lab Clean Energy, Dalian Inst Chem Phys, Dalian 116023, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
3.Dalian Univ Technol, State Key Lab Fine Chem, PSU DUT Joint Ctr Energy Res, Sch Chem Engn, Dalian 116024, Peoples R China
Recommended Citation
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.
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