Observation of an oxonium ion intermediate in ethanol dehydration to ethene on zeolite

doi:10.1038/s41467-019-09956-7

	Observation of an oxonium ion intermediate in ethanol dehydration to ethene on zeolite
	Deng, Feng 3; Feng, Ningdong 3; Zhao, Xingling 2,3; Qi, Guodong 3; Wang, Qiang 3; Xu, Jun 1,3; Chu, Yueying 3; Wang, Chao 3; Zhou, Xue 2,3
刊名	NATURE COMMUNICATIONS
	2019-04-29
卷号	10 页码:9
ISSN号	2041-1723
DOI	10.1038/s41467-019-09956-7
英文摘要	Zeolite-catalyzed dehydration of ethanol offers promising perspectives for the sustainable production of ethene. Complex parallel-consecutive pathways are proposed to be involved in the reaction network of ethanol dehydration on zeolites, where the initial step of ethanol dehydration is still unclear particularly for the favorable production of ethene at lower temperature. Here we report the observation of a triethyloxonium ion (TEO) in the dehydration of ethanol on zeolite H-ZSM-5 by using ex situ and in situ solid-state NMR spectroscopy. TEO is identified as a stable surface species on the working catalyst, which shows high reactivity during reaction. Ethylation of the zeolite by TEO occurs at lower temperature, leading to the formation of surface ethoxy species and then ethene. The TEO-ethoxide pathway is found to be energetically preferable for the dehydration of ethanol to ethene in the initial stage, which is also supported by theoretical calculations.
资助项目	National Natural Science Foundation of China[21622311] ; National Natural Science Foundation of China[21473245] ; National Natural Science Foundation of China[21603265] ; National Natural Science Foundation of China[21733013] ; National Natural Science Foundation of China[21773296] ; key program for frontier science of the Chinese Academy of Sciences[QYZDB-SSW-SLH027] ; Hubei Provincial Natural Science Foundation[2017CFA032]
WOS关键词	TO-GASOLINE CHEMISTRY ; OLEFINS CONVERSION ; METHANOL ; HYDROCARBONS ; H-ZSM-5 ; MECHANISM ; ETHYLENE ; DECOMPOSITION ; SPECTROSCOPY ; COMPLEXES
WOS研究方向	Science & Technology - Other Topics
语种	英语
出版者	NATURE PUBLISHING GROUP
WOS记录号	WOS:000466120200005
资助机构	National Natural Science Foundation of China ; National Natural Science Foundation of China ; key program for frontier science of the Chinese Academy of Sciences ; key program for frontier science of the Chinese Academy of Sciences ; Hubei Provincial Natural Science Foundation ; Hubei Provincial Natural Science Foundation ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; key program for frontier science of the Chinese Academy of Sciences ; key program for frontier science of the Chinese Academy of Sciences ; Hubei Provincial Natural Science Foundation ; Hubei Provincial Natural Science Foundation ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; key program for frontier science of the Chinese Academy of Sciences ; key program for frontier science of the Chinese Academy of Sciences ; Hubei Provincial Natural Science Foundation ; Hubei Provincial Natural Science Foundation ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; key program for frontier science of the Chinese Academy of Sciences ; key program for frontier science of the Chinese Academy of Sciences ; Hubei Provincial Natural Science Foundation ; Hubei Provincial Natural Science Foundation
内容类型	期刊论文
源URL	[http://ir.wipm.ac.cn/handle/112942/13706]
专题	中国科学院武汉物理与数学研究所
通讯作者	Deng, Feng; Xu, Jun
作者单位	1.Huazhong Univ Sci & Technol, Wuhan Natl Lab Optoelect, Wuhan 430074, Hubei, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 3.Chinese Acad Sci, Wuhan Inst Phys & Math, Natl Ctr Magnet Resonance Wuhan,Key Lab Magnet Re, State Key Lab Magnet Resonance & Atom & Mol Phys, Wuhan 430071, Hubei, Peoples R China
推荐引用方式 GB/T 7714	Deng, Feng,Feng, Ningdong,Zhao, Xingling,et al. Observation of an oxonium ion intermediate in ethanol dehydration to ethene on zeolite[J]. NATURE COMMUNICATIONS,2019,10:9.
APA	Deng, Feng.,Feng, Ningdong.,Zhao, Xingling.,Qi, Guodong.,Wang, Qiang.,...&Zhou, Xue.(2019).Observation of an oxonium ion intermediate in ethanol dehydration to ethene on zeolite.NATURE COMMUNICATIONS,10,9.
MLA	Deng, Feng,et al."Observation of an oxonium ion intermediate in ethanol dehydration to ethene on zeolite".NATURE COMMUNICATIONS 10(2019):9.