Slight channel difference influences the reaction pathway of methanol-to-olefins conversion over acidic H-ZSM-22 and H-ZSM-12 zeolites

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

	Slight channel difference influences the reaction pathway of methanol-to-olefins conversion over acidic H-ZSM-22 and H-ZSM-12 zeolites
	Chu, Yueying 1; Sun, Xianyong 2; Yi, Xianfeng 1; Ding, Lihong 1; Zheng, Anmin 1,3; Deng, Feng 1
刊名	CATALYSIS SCIENCE & TECHNOLOGY
	2015
卷号	5 期号:7 页码:3507-3517
英文摘要	The methanol to olefins (MTO) process, in which low-value carbon-rich feedstocks are converted to value-added petrochemical products, is one of the most prominent alternatives for the production of light olefins. In order to reveal the confinement effect of zeolites on the catalytic reactions, the MTO mechanisms and reactivity over two unidimensional zeolites (H-ZSM-12 and H-ZSM-22) with a channel difference of only 0.3 angstrom have been systematically explored by DFT calculations in this work. The calculated activation barriers and reaction energies demonstrated that the 0.3 angstrom channel difference between H-ZSM-12 and H-ZSM-22 zeolites results in a dramatic discrepancy in their transition state selectivity associated with the aromatic-based hydrocarbon pool (HCP) mechanism. For the larger H-ZSM-12 zeolite, the formation of pentamethybenzenium cation was favored, which would be the active HCP species in the MTO reaction. For the H-ZSM-22 zeolite with a 0.3 angstrom smaller pore structure, the traditional methylation at the C-H sites of polymethylbenzenes occurred exclusively. When the alternative olefin-based cycle is followed for the MTO reaction, both of the zeolites are active catalysts for the formations of butene and propene. A comparison of the activation barriers for the olefin-based cycle revealed that the larger H-ZSM-12 possesses a higher catalytic activity than the H-ZSM-22 zeolite. Our theoretical results demonstrate that both the aromatic-based cycle and the olefin-based cycle can proceed during the MTO reaction over H-ZSM-12, with the latter cycle being predominant.
WOS标题词	Science & Technology ; Physical Sciences
类目[WOS]	Chemistry, Physical
研究领域[WOS]	Chemistry
关键词[WOS]	DENSITY-FUNCTIONAL THEORY ; REACTION-MECHANISM ; HYDROCARBONS CONVERSION ; CATALYTIC CYCLE ; CARBENIUM IONS ; CO-REACTION ; METHYLATION ; SELECTIVITY ; INSIGHTS ; SAPO-34
收录类别	SCI
语种	英语
WOS记录号	WOS:000356610600008
公开日期	2015-07-28
内容类型	期刊论文
源URL	[http://ir.wipm.ac.cn/handle/112942/4767]
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, Peoples R China 2.Coal Chem Catalysis Ctr, Natl Inst Clean & Low Carbon Energy NICE, Beijing 102211, Peoples R China 3.Huanggang Normal Univ, Hubei Key Lab Proc & Applicat Catalyt Mat, Huanggang 438000, Hubei, Peoples R China
推荐引用方式 GB/T 7714	Chu, Yueying,Sun, Xianyong,Yi, Xianfeng,et al. Slight channel difference influences the reaction pathway of methanol-to-olefins conversion over acidic H-ZSM-22 and H-ZSM-12 zeolites[J]. CATALYSIS SCIENCE & TECHNOLOGY,2015,5(7):3507-3517.
APA	Chu, Yueying,Sun, Xianyong,Yi, Xianfeng,Ding, Lihong,Zheng, Anmin,&Deng, Feng.(2015).Slight channel difference influences the reaction pathway of methanol-to-olefins conversion over acidic H-ZSM-22 and H-ZSM-12 zeolites.CATALYSIS SCIENCE & TECHNOLOGY,5(7),3507-3517.
MLA	Chu, Yueying,et al."Slight channel difference influences the reaction pathway of methanol-to-olefins conversion over acidic H-ZSM-22 and H-ZSM-12 zeolites".CATALYSIS SCIENCE & TECHNOLOGY 5.7(2015):3507-3517.