Impact of temporal and spatial distribution of hydrocarbon pool on methanol conversion over H-ZSM-5

doi:10.1016/j.jcat.2017.08.003

CORC > 武汉物理与数学研究所 > 中国科学院武汉物理与数学研究所 > 磁共振应用研究部

	Impact of temporal and spatial distribution of hydrocarbon pool on methanol conversion over H-ZSM-5
	Wang, Chao 1; Wang, Qiang 1; Li, Wenzheng 1; Zhao, Xingling 1; Wang, Weiyu 1; Qi, Guodong 1; Xu, Jun 1; Sun, Xianyong 2; Deng, Feng 1
刊名	JOURNAL OF CATALYSIS
	2017-10-01
卷号	354 页码:138-151
关键词	Hydrocarbon Pool Olefins Zeolite Mechanism Nmr Spectroscopy
DOI	10.1016/j.jcat.2017.08.003
文献子类	Article
英文摘要	The hydrocarbon pool (HP) species in methanol-to-olefins (MTO) reactions over zeolite H-ZSM-5 were investigated by solid-state NMR spectroscopy and GC-MS. The distribution and reactivity of retained HP species such as carbocations and methylbenzenes (MBs) were found to evolve with reaction time and their positions in the catalyst bed. The underlying mechanism of the typical S-shaped methanol conversion curve was revealed, in which the dominating reaction route was found to be dependent on the formation and reactivity of different HP species that were varied at different reaction time. During the induction period, cyclopentenyl cations served as the precursor to MBs and exhibited higher reactivity than the latter. The reaction was accelerated by the accumulation of alkenes and further enhanced by consequent involvement of the cyclopentenyl cations and aromatics, which eventually led to a steady state reaction. The interconversions of the reaction cycles based on alkenes, cyclopentenyl cations, and MBs were proposed for the formation of light olefins. The co-catalysis of HP species in the MTO reactions showed that the cyclopentenyl cations and alkenes favored propene formation, while the light MBs such as xylene and triMB facilitated ethene formation. Within the catalyst bed, both cyclopentenyl cations and MBs were dominantly formed in the upper catalyst layers. The experiments indicated that both cyclopentenyl cations and alkenes maintained high reactivity throughout the catalytic bed, while MBs exhibited high reactivity only in the upper catalyst position. (C) 2017 Elsevier Inc. All rights reserved.
WOS关键词	ACIDIC ZEOLITE CATALYSTS ; STATE NMR-SPECTROSCOPY ; TO-OLEFINS CONVERSION ; SURFACE METHOXY GROUPS ; AROMATIC-HYDROCARBONS ; H-BETA ; HEPTAMETHYLBENZENIUM CATION ; PRODUCT SELECTIVITY ; REACTION-MECHANISM ; COKE FORMATION
WOS研究方向	Chemistry ; Engineering
语种	英语
WOS记录号	WOS:000413283000013
资助机构	National Natural Science Foundation of China(21622311 ; National Natural Science Foundation of China(21622311 ; key program for frontier science of the Chinese Academy of Sciences(QYZDB-SSW-SLH027) ; key program for frontier science of the Chinese Academy of Sciences(QYZDB-SSW-SLH027) ; 21611130104 ; 21611130104 ; 21473245 ; 21473245 ; 21210005) ; 21210005) ; National Natural Science Foundation of China(21622311 ; National Natural Science Foundation of China(21622311 ; key program for frontier science of the Chinese Academy of Sciences(QYZDB-SSW-SLH027) ; key program for frontier science of the Chinese Academy of Sciences(QYZDB-SSW-SLH027) ; 21611130104 ; 21611130104 ; 21473245 ; 21473245 ; 21210005) ; 21210005)
内容类型	期刊论文
源URL	[http://ir.wipm.ac.cn/handle/112942/11429]
专题	武汉物理与数学研究所_磁共振应用研究部
作者单位	1.Chinese Acad Sci, Wuhan Inst Phys & Math, Natl Ctr Magnet Resonance Wuhan, State Key Lab Magnet Resonance & Atom & Mol Phys, Wuhan 430071, Hubei, Peoples R China 2.Natl Inst Clean & Low Carbon Energy, Beijing 102211, Peoples R China
推荐引用方式 GB/T 7714	Wang, Chao,Wang, Qiang,Li, Wenzheng,et al. Impact of temporal and spatial distribution of hydrocarbon pool on methanol conversion over H-ZSM-5[J]. JOURNAL OF CATALYSIS,2017,354:138-151.
APA	Wang, Chao.,Wang, Qiang.,Li, Wenzheng.,Zhao, Xingling.,Wang, Weiyu.,...&Deng, Feng.(2017).Impact of temporal and spatial distribution of hydrocarbon pool on methanol conversion over H-ZSM-5.JOURNAL OF CATALYSIS,354,138-151.
MLA	Wang, Chao,et al."Impact of temporal and spatial distribution of hydrocarbon pool on methanol conversion over H-ZSM-5".JOURNAL OF CATALYSIS 354(2017):138-151.