New Insights into the Effects of Acid Strength on the Solid Acid-Catalyzed Reaction: Theoretical Calculation Study of Olefinic Hydrocarbon Protonation Reaction

CORC > 武汉物理与数学研究所 > 中国科学院武汉物理与数学研究所 > 2011年以前论文发表（包括2011年）

	New Insights into the Effects of Acid Strength on the Solid Acid-Catalyzed Reaction: Theoretical Calculation Study of Olefinic Hydrocarbon Protonation Reaction
	Fang, Hanjun 1,2; Zheng, Anmin 1; Li, Shenhui 1; Xu, Jun 1; Chen, Lei 1; Deng, Feng 1
刊名	JOURNAL OF PHYSICAL CHEMISTRY C
	2010-06-10
卷号	114 期号:22 页码:10254-10264
产权排序	第一
英文摘要	The protonation reactions of propene, isobutene, styrene, and a-methylstyrene on 8T solid acid models with varying acid strengths are theoretically studied in order to reveal the effects of acid strength on the solid acid-catalyzed reactions. It is shown that with the increase of acid strength (evaluated by deprotonation energy) the ion pair intermediates are preferentially formed, and their stabilities relative to the pi complex and alkoxy species intermediates are considerably increased. Some alkoxy species for the bulkier olefinic hydrocarbons (i.e., isobutene, styrene, and a-methylstyrene) cannot exist as stable intermediates on strong solid acid models. It is further found that with the increase of acid strength the extent of energy reduction generally follows the order of ion pair > transition states (TS, TS') > (pi complex, alkoxy species), which is in line with the ionic character of these species. The ionic species are much more sensitive to acid strength than the covalent species regardless of intermediates or transition states. This can explain the increase of the stability of ion pair intermediates on strong solid acid models. In addition, the results obtained here can be used to interpret the effects of acid strength on the catalytic activities for other solid acid-catalyzed reactions, such as alkanol dehydration, alkane isomerization, and Beckmann rearrangement.
学科主题	波谱分析
WOS标题词	Science & Technology ; Physical Sciences ; Technology
类目[WOS]	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 ; TERT-BUTYL CATION ; DENSITY-FUNCTIONAL THEORY ; CARBENIUM IONS ; AB-INITIO ; CHEMICAL-SHIFT ; BECKMANN REARRANGEMENT ; SKELETAL ISOMERIZATION ; CONVERSION REACTIONS ; ALUMINUM-CHLORIDE
收录类别	SCI
语种	英语
WOS记录号	WOS:000278301200024
内容类型	期刊论文
源URL	[http://ir.wipm.ac.cn/handle/112942/1973]
专题	武汉物理与数学研究所_2011年以前论文发表（包括2011年）
作者单位	1.Chinese Acad Sci, Wuhan Inst Phys & Math, Wuhan Ctr Magnet Resonance, State Key Lab Magnet Resonance & Atom & Mol Phys, 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	Fang, Hanjun,Zheng, Anmin,Li, Shenhui,et al. New Insights into the Effects of Acid Strength on the Solid Acid-Catalyzed Reaction: Theoretical Calculation Study of Olefinic Hydrocarbon Protonation Reaction[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2010,114(22):10254-10264.
APA	Fang, Hanjun,Zheng, Anmin,Li, Shenhui,Xu, Jun,Chen, Lei,&Deng, Feng.(2010).New Insights into the Effects of Acid Strength on the Solid Acid-Catalyzed Reaction: Theoretical Calculation Study of Olefinic Hydrocarbon Protonation Reaction.JOURNAL OF PHYSICAL CHEMISTRY C,114(22),10254-10264.
MLA	Fang, Hanjun,et al."New Insights into the Effects of Acid Strength on the Solid Acid-Catalyzed Reaction: Theoretical Calculation Study of Olefinic Hydrocarbon Protonation Reaction".JOURNAL OF PHYSICAL CHEMISTRY C 114.22(2010):10254-10264.