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题名: Interactions of phosphorous molecules with the acid sites of H-Beta zeolite: Insights from solid-state NMR techniques and theoretical calculations
作者: Guan, Jing1;  Li, Xiujie1;  Yang, Gang1;  Zhang, Weiping1;  Liu, Xianchun1;  Han, Xiuwen1;  Bao, Xinhe1
通讯作者: 包信和
关键词: Solid-state NMR technique ;  Theoretical calculations ;  Bronsted acids ;  Lewis acids ;  Probe molecule
刊名: JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL
发表日期: 2009-09-01
DOI: 10.1016/j.molcata.2009.06.005
卷: 310, 期:1-2, 页:113-120
收录类别: SCI
文章类型: Article
部门归属: 5,8
项目归属: 502,802
产权排名: 1;1
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Chemistry, Physical
研究领域[WOS]: Chemistry
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.
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
语种: 英语
原文出处: 查看原文
WOS记录号: WOS:000269426900014
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/102313
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China

Recommended Citation:
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.
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