Mechanism of alkane H/D exchange over zeolite H-ZSM-5 at low temperature: a combined computational and experimental study

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	Mechanism of alkane H/D exchange over zeolite H-ZSM-5 at low temperature: a combined computational and experimental study
	Chu, Yueying 1; Xue, Nianhua 2; Xu, Bolian 2; Ding, Qian 3,4; Feng, Zhaochi 3; Zheng, Anmin 1; Deng, Feng 1
刊名	CATALYSIS SCIENCE & TECHNOLOGY
	2016
卷号	6 期号:14 页码:5350-5363
英文摘要	Theoretical calculations have provided fundamental insights into the possible pathways for the H/D exchange of isobutane with H-ZSM-5 zeolite at room temperature. It is theoretically demonstrated that neither the direct exchange mechanism nor the indirect bimolecular hydride transfer mechanism is an efficient route for isobutane activation due to high activation barriers, which possibly prohibit H/D exchange at low temperatures. It is revealed that a trace of olefin impurities can considerably accelerate the formation of an alkoxyl intermediate which is involved in the bimolecular hydride transfer mechanism. Once the alkoxyl intermediate is generated from the olefin impurities, the catalytic cycle is self-sustaining. On the other hand, the theoretical calculations also illustrate that the extra-framework aluminum (EFAl) species in the dealuminated zeolite has no obvious promotional effect on the H/D exchange. Furthermore, our calculations are also consistent with the experimental results.
WOS标题词	Science & Technology ; Physical Sciences
类目[WOS]	Chemistry, Physical
研究领域[WOS]	Chemistry
关键词[WOS]	EXTRA-FRAMEWORK ALUMINUM ; SOLID-STATE NMR ; DENSITY-FUNCTIONAL THEORY ; H BOND ACTIVATION ; HYDRIDE TRANSFER ; EXTRAFRAMEWORK ALUMINUM ; THEORETICAL CALCULATION ; SULFATED ZIRCONIA ; ZSM-5 ZEOLITE ; HIGH-FIELD
收录类别	SCI
语种	英语
WOS记录号	WOS:000379438000011
内容类型	期刊论文
源URL	[http://ir.wipm.ac.cn/handle/112942/9462]
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, State Key Lab Magnet Resonance & Atom & Mol Phys, Natl Ctr Magnet Resonance Wuhan, Wuhan Inst Phys & Math, Wuhan 430071, Peoples R China 2.Nanjing Univ, Key Lab Mesoscop Chem, Sch Chem & Chem Engn, Nanjing 210093, Jiangsu, Peoples R China 3.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China 4.Chinese Acad Sci, Grad Univ, Beijing 100864, Peoples R China
推荐引用方式 GB/T 7714	Chu, Yueying,Xue, Nianhua,Xu, Bolian,et al. Mechanism of alkane H/D exchange over zeolite H-ZSM-5 at low temperature: a combined computational and experimental study[J]. CATALYSIS SCIENCE & TECHNOLOGY,2016,6(14):5350-5363.
APA	Chu, Yueying.,Xue, Nianhua.,Xu, Bolian.,Ding, Qian.,Feng, Zhaochi.,...&Deng, Feng.(2016).Mechanism of alkane H/D exchange over zeolite H-ZSM-5 at low temperature: a combined computational and experimental study.CATALYSIS SCIENCE & TECHNOLOGY,6(14),5350-5363.
MLA	Chu, Yueying,et al."Mechanism of alkane H/D exchange over zeolite H-ZSM-5 at low temperature: a combined computational and experimental study".CATALYSIS SCIENCE & TECHNOLOGY 6.14(2016):5350-5363.