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

文献类型：期刊论文

作者Deng, Feng3; Feng, Ningdong3; Zhao, Xingling2,3; Qi, Guodong3; Wang, Qiang3; Xu, Jun1,3; Chu, Yueying3; Wang, Chao3; Zhou, Xue2,3
刊名NATURE COMMUNICATIONS
出版日期2019-04-29
卷号10页码:9
ISSN号2041-1723
DOI10.1038/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.
WOS关键词TO-GASOLINE CHEMISTRY ; OLEFINS CONVERSION ; METHANOL ; HYDROCARBONS ; H-ZSM-5 ; MECHANISM ; ETHYLENE ; DECOMPOSITION ; SPECTROSCOPY ; COMPLEXES
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研究方向Science & Technology - Other Topics
语种英语
WOS记录号WOS:000466120200005
出版者NATURE PUBLISHING GROUP
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
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.

入库方式： OAI收割

来源：武汉物理与数学研究所

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