Carbonylation of ethane with carbon monoxide over Zn-modified ZSM-5 zeolites studied by in situ solid-state NMR spectroscopy

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	Carbonylation of ethane with carbon monoxide over Zn-modified ZSM-5 zeolites studied by in situ solid-state NMR spectroscopy
	Wang, Xiumei; Xu, Jun; Qi, Guodong; Wang, Chao; Wang, Weiyu; Gao, Pan; Wang, Qiang; Liu, Xiaolong; Feng, Ningdong; Deng, Feng
刊名	JOURNAL OF CATALYSIS
	2017
卷号	345 页码:228-235
关键词	Light alkane activation Carbonylation MAS NMR spectroscopy Reaction mechanism Zeolites
英文摘要	The carbonylation reaction of ethane with CO to produce carboxylic acid was studied over zinc-modified ZSM-5 zeolite (denoted as Zn/ZSM-5) using in situ solid-state NMR spectroscopy. C-13-isotope-labeled reactants were alternatively used to monitor the co-reaction at temperatures of 298-623 K. The NMR experimental results demonstrated that surface zinc-ethyl and methoxy species were formed and identified as key intermediates in the reaction. The reactivity of these intermediates was further explored under both oxidizing and reducing conditions by adding O-2 and H-2 into the reaction system. It was found that ethane was initially activated into zinc-ethyl species that show reactivity similar to that of organometallic compounds such as diethyl zinc. The interaction of zinc-ethyl species with CO2 resulting from the oxidation of CO produces propanoic acid. Side products such as aromatics were formed by dehydrogenation of zinc-ethyl species via the formed ethene intermediates. We also found that hydrogenolysis of ethane occurred and gave rise to byproduct methane, which led to the formation of acetic acid by carboxylation with CO2. Additionally, CO was converted into surface methoxy species, which could react with CO to produce acetic acid via a Koch-type carbonylation reaction. (C) 2016 Elsevier Inc. All rights reserved.
WOS标题词	Science & Technology ; Physical Sciences ; Technology
类目[WOS]	Chemistry, Physical ; Engineering, Chemical
研究领域[WOS]	Chemistry ; Engineering
关键词[WOS]	PROMOTED H-ZSM-5 CATALYSTS ; ACETIC-ACID ; DIMETHYL ETHER ; DISSOCIATIVE ADSORPTION ; SATURATED-HYDROCARBONS ; PROPANE AROMATIZATION ; ORGANOZINC REAGENTS ; SELECTIVE OXIDATION ; METHANE ADSORPTION ; CARBOXYLIC-ACIDS
收录类别	SCI
语种	英语
WOS记录号	WOS:000393529600020
内容类型	期刊论文
源URL	[http://ir.wipm.ac.cn/handle/112942/10034]
专题	武汉物理与数学研究所_磁共振应用研究部
作者单位	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
推荐引用方式 GB/T 7714	Wang, Xiumei,Xu, Jun,Qi, Guodong,et al. Carbonylation of ethane with carbon monoxide over Zn-modified ZSM-5 zeolites studied by in situ solid-state NMR spectroscopy[J]. JOURNAL OF CATALYSIS,2017,345:228-235.
APA	Wang, Xiumei.,Xu, Jun.,Qi, Guodong.,Wang, Chao.,Wang, Weiyu.,...&Deng, Feng.(2017).Carbonylation of ethane with carbon monoxide over Zn-modified ZSM-5 zeolites studied by in situ solid-state NMR spectroscopy.JOURNAL OF CATALYSIS,345,228-235.
MLA	Wang, Xiumei,et al."Carbonylation of ethane with carbon monoxide over Zn-modified ZSM-5 zeolites studied by in situ solid-state NMR spectroscopy".JOURNAL OF CATALYSIS 345(2017):228-235.