Interactions of phosphorous molecules with the acid sites of H-Beta zeolite: Insights from solid-state NMR techniques and theoretical calculations

	Interactions of phosphorous molecules with the acid sites of H-Beta zeolite: Insights from solid-state NMR techniques and theoretical calculations
	Guan, Jing; Li, Xiujie; Yang, Gang; Zhang, Weiping; Liu, Xianchun; Han, Xiuwen; Bao, Xinhe
刊名	journal of molecular catalysis a-chemical
	2009-09-01
卷号	310 期号:1-2 页码:113-120
关键词	Solid-state NMR technique Theoretical calculations Bronsted acids Lewis acids Probe molecule
通讯作者	包信和
产权排序	1;1
英文摘要	the local structures of various bronsted and lewis acid sites in h-beta zeolite were resolved with the combined (31)p mas nmr, (31)p-(27)al trapdor nmr experiments and theoretical calculations at different levels. in addition, the interacting mechanisms of these acid sites with probe molecules such as trimethylphosphine (tmp) and trimethylphosphine oxide (tmpo) were clarified,which greatly aids the understanding of acid catalysis. owing to the narrow chemical shift range and close bronsted acid strengths, only an average resonance at -4.5 ppm was observed in tmp adsorbed h-beta zeolite, consistent with the calculated data of acidities (substitution energies and proton affinities), geometries, adsorption energies as well as (31)p chemical shifts. however, two types of bronsted acids were distinguished by tmpo, and the hf/dzvp2 (mp2/dzvp2) chemical shifts were calculated at 68.1 (69.5) and 69.7-72.1 (71.7-74.9)ppm, respectively. two types of lewis acids were identified at -32.0 and -47.0 ppm with the latter exhibiting strong (31)p-(27)al trapdor effects. with theoretical calculations, these two peaks were attributed to the extra-lattice oxo-aloh(2+) species and the three-fold coordinated lattice-al, extra-framework al(oh)(3), oxo-alo(+) species, respectively. the peak at -60.0 ppm was conventionally assigned to the tmp physisorption, but the calculations indicated that the efal monovalent al(oh)(2)(+) species coordinating with two lattice-o atoms near the framework all atom can contribute to it as well. (c) 2009 published by elsevier b.v.
WOS标题词	science & technology ; physical sciences
类目[WOS]	chemistry, physical
研究领域[WOS]	chemistry
关键词[WOS]	density-functional theory ; trimethylphosphine oxide ; chemical-shifts ; probe molecule ; p-31 nmr ; mas nmr ; olefin metathesis ; double-resonance ; y-zeolite ; catalysts
收录类别	SCI
原文出处	false
语种	英语
WOS记录号	WOS:000269426900014
公开日期	2010-11-30
内容类型	期刊论文
源URL	[http://159.226.238.44/handle/321008/102313]
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
作者单位	Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
推荐引用方式 GB/T 7714	Guan, Jing,Li, Xiujie,Yang, Gang,et al. Interactions of phosphorous molecules with the acid sites of H-Beta zeolite: Insights from solid-state NMR techniques and theoretical calculations[J]. journal of molecular catalysis a-chemical,2009,310(1-2):113-120.
APA	Guan, Jing.,Li, Xiujie.,Yang, Gang.,Zhang, Weiping.,Liu, Xianchun.,...&Bao, Xinhe.(2009).Interactions of phosphorous molecules with the acid sites of H-Beta zeolite: Insights from solid-state NMR techniques and theoretical calculations.journal of molecular catalysis a-chemical,310(1-2),113-120.
MLA	Guan, Jing,et al."Interactions of phosphorous molecules with the acid sites of H-Beta zeolite: Insights from solid-state NMR techniques and theoretical calculations".journal of molecular catalysis a-chemical 310.1-2(2009):113-120.