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题名: Elucidating the olefin formation mechanism in the methanol to olefin reaction over AlPO-18 and SAPO-18
作者: Chen, Jingrun1, 2;  Li, Jinzhe1;  Yuan, Cuiyu1;  Xu, Shutao1;  Wei, Yingxu1;  Wang, Quanyi1, 2;  Zhou, You1, 2;  Wang, Jinbang1, 2;  Zhang, Mozhi1, 2;  He, Yanli1;  Xu, Shuliang1;  Liu, Zhongmin1
刊名: CATALYSIS SCIENCE & TECHNOLOGY
发表日期: 2014
DOI: 10.1039/c4cy00551a
卷: 4, 期:9, 页:3268-3277
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Chemistry, Physical
研究领域[WOS]: Chemistry
英文摘要: The mechanism of the methanol to olefin (MTO) reaction over AlPO-18 (without Bronsted acid sites) and two SAPO-18 (with different Bronsted acid site densities) catalysts has been investigated. The Bronsted acid site density of AlPO-18 and SAPO-18 catalysts was determined by H-1 MAS NMR spectroscopy. Methanol conversion over the catalysts showed that the catalytic activity of the catalysts was strongly influenced by their Bronsted acid site density. Using C-13 magic angle spinning (MAS) NMR, we directly observed the pentamethylcyclopentenyl cation (pentaMCP(+)) over SAPO-18 under real MTO reaction conditions, but no carbenium ion was detected over AlPO-18. Furthermore, analysis of confined organics by C-13 MAS NMR and GC-MS clearly demonstrated that higher Bronsted acid site density improved the formation and accumulation of some important and reactive hydrocarbon pool species, such as pentaMCP(+) and polymethylbenzenes. With the aid of the C-12/C-13-methanol switch technique, the detailed olefin formation mechanism was elucidated. During the MTO reaction, light olefin generation over SAPO-18 mainly followed the aromatic-based hydrocarbon pool mechanism; however, the olefin methylation and cracking mechanism accounted for the production of light olefins over AlPO-18.
关键词[WOS]: TO-HYDROCARBONS REACTION ;  BRONSTED ACID SITES ;  CATALYTIC CYCLE ;  CARBENIUM IONS ;  HEPTAMETHYLBENZENIUM CATION ;  PRODUCT SELECTIVITY ;  ZEOLITE H-ZSM-5 ;  COKE FORMATION ;  CONVERSION ;  HSAPO-34
语种: 英语
WOS记录号: WOS:000340208400056
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/145564
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Natl Engn Lab Methanol Olefins, Dalian 116023, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China

Recommended Citation:
Chen, Jingrun,Li, Jinzhe,Yuan, Cuiyu,et al. Elucidating the olefin formation mechanism in the methanol to olefin reaction over AlPO-18 and SAPO-18[J]. CATALYSIS SCIENCE & TECHNOLOGY,2014,4(9):3268-3277.
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