Influence of acid strength on the reactivity of alkane activation on solid acid catalysts: A theoretical calculation study

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	Influence of acid strength on the reactivity of alkane activation on solid acid catalysts: A theoretical calculation study
	Chu, Yueying 1,2; Han, Bing 1,2; Fang, Hanjun 1; Zheng, Anmin 1; Deng, Feng 1
刊名	MICROPOROUS AND MESOPOROUS MATERIALS
	2012-03-15
卷号	151 页码:241-249
关键词	Density functional theory Deprotonation energy Activation energy Rate constant Reaction acidic sensitivity
英文摘要	The influence of Bronsted acid strength on the reactivities of alkane activations has been systematically studied by density functional theory (OFT) calculations. Some typical reactions, such as methane hydrogen exchange (C-H bond activation), propane dehydrogenation (C-H bond dissociation and H-H bond formation), and propane cracking (C-C cleavage), were investigated on 8T solid acid models with varying acid strengths from weak-, strong-, to super-acid. According to our calculational results, it was revealed that the activation barriers (E-act) of all the reactions decrease linearly, while the rate coefficients (log k) increase linearly with increasing the acid strength, being indicative of the enhancement of reactivities. However, the reactivity of different reactions exhibits different sensitivity to acid strength: the propane cracking is most sensitive to acid strength, while the methane hydrogen exchange reaction is least sensitive to acid strength. On the basis of the natural charge on the organic fragment in the transition state, it was revealed that the sensitivity of the reactivity to acid strength could be related to the ionic character of the transition state. The propane cracking reaction possesses a more ionic transition state (0.913-0.964 vertical bar e vertical bar), while the methane hydrogen exchange has a less ionic transition state (0.646-0.773 vertical bar e vertical bar). (C) 2011 Elsevier Inc. All rights reserved.
WOS标题词	Science & Technology ; Physical Sciences ; Technology
类目[WOS]	Chemistry, Applied ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary
研究领域[WOS]	Chemistry ; Science & Technology - Other Topics ; Materials Science
关键词[WOS]	STATE NMR-SPECTROSCOPY ; C-13 CHEMICAL-SHIFT ; AB-INITIO ; CONVERSION REACTIONS ; VIBRATIONAL ANALYSIS ; KEGGIN 12-H3PW12O40 ; EXCHANGE-REACTIONS ; CRACKING REACTIONS ; HYDROGEN-EXCHANGE ; ZEOLITE CATALYSIS
收录类别	SCI
语种	英语
WOS记录号	WOS:000300747000030
公开日期	2015-07-14
内容类型	期刊论文
源URL	[http://ir.wipm.ac.cn/handle/112942/1704]
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, Wuhan Ctr Magnet Resonance, Wuhan Inst Phys & Math, Wuhan 430071, Peoples R China 2.Chinese Acad Sci, Grad Sch, Beijing 100049, Peoples R China
推荐引用方式 GB/T 7714	Chu, Yueying,Han, Bing,Fang, Hanjun,et al. Influence of acid strength on the reactivity of alkane activation on solid acid catalysts: A theoretical calculation study[J]. MICROPOROUS AND MESOPOROUS MATERIALS,2012,151:241-249.
APA	Chu, Yueying,Han, Bing,Fang, Hanjun,Zheng, Anmin,&Deng, Feng.(2012).Influence of acid strength on the reactivity of alkane activation on solid acid catalysts: A theoretical calculation study.MICROPOROUS AND MESOPOROUS MATERIALS,151,241-249.
MLA	Chu, Yueying,et al."Influence of acid strength on the reactivity of alkane activation on solid acid catalysts: A theoretical calculation study".MICROPOROUS AND MESOPOROUS MATERIALS 151(2012):241-249.