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

doi:10.1039/c6cy00467a

	Mechanism of alkane H/D exchange over zeolite H-ZSM-5 at low temperature: a combined computational and experimental study
	Xue, Nianhua 3; Xu, Bolian 3; Ding, Qian 1,4; Feng, Zhaochi 1; Chu, Yueying 2; Zheng, Anmin 2; Deng, Feng 2
刊名	CATALYSIS SCIENCE & TECHNOLOGY
	2016
卷号	6 期号:14 页码:5350-5363
ISSN号	2044-4753
DOI	10.1039/c6cy00467a
文献子类	Article
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关键词	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
WOS研究方向	Chemistry
语种	英语
出版者	ROYAL SOC CHEMISTRY
WOS记录号	WOS:000379438000011
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/170358]
专题	大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者	Zheng, Anmin; Deng, Feng
作者单位	1.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China 2.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 3.Nanjing Univ, Key Lab Mesoscop Chem, Sch Chem & Chem Engn, Nanjing 210093, Jiangsu, Peoples R China 4.Chinese Acad Sci, Grad Univ, Beijing 100864, Peoples R China
推荐引用方式 GB/T 7714	Xue, Nianhua,Xu, Bolian,Ding, Qian,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	Xue, Nianhua.,Xu, Bolian.,Ding, Qian.,Feng, Zhaochi.,Chu, Yueying.,...&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	Xue, Nianhua,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.