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题名: DFT studies on the location and acid strength of Bronsted acid sites in MCM-22 zeolite
作者: Zhou, DH;  Bao, Y;  Yang, MM;  He, N;  Yang, G
通讯作者: Zhou DH
关键词: DFT calculations ;  MCM-22 zeolite ;  Al substitution ;  Bronsted acid site ;  acidity
刊名: JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL
发表日期: 2006-02-01
DOI: 10.1016/j.molcata.2005.08.034
卷: 244, 期:1-2, 页:11-19
收录类别: SCI
文章类型: Article
部门归属: 5
项目归属: 502
产权排名: 2;1
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Chemistry, Physical
研究领域[WOS]: Chemistry
英文摘要: Density functional theory was applied to study the location and the acid strength of Bronsted acid sites in MCM-22 zeolite. The calculations were performed based on cluster model by using of B3LYP hydride functional and 6-31G** basis set. The replacements of Si by Al at eight inequivalent tetrahedral crystallographic sites and the corresponding Si(OH)A1 sites were examined by calculating the (A1,H)/Si substitution energy, deprotonation energy, hydroxyl stretching vibtational frequency and the adsorption energy of some basic probe molecules on the acid centers. According to the calculated results it was predicated that the most favorable sites for framework Al substitutions in MCM-22 were T1, T3, and T4 sites and the most preferable Bronsted acid sites were oil A11(O3H)Si4, A14(O3H)Si1, and A13(O11H)Si2 bridged groups. The first two acid sites located on the 12-membered ring in the supercages, and the third located in the 10-membered ring sinusoidal channels. Evaluating of acid strength by the calculated ammonia adsorption energies revealed that A11(O3H)Si4 and A14(O3H)Si1 sites display the similar acidity, and that stronger than A13(O11H)Si2. The calculated hydroxyl vibrational frequencies of three acid sites were 3628 cm(-1), 3618 cm(-1), and 3592 cm(-1)(corrected with scaling factor 0.948), respectively, consistent with the reported FTIR experimental data. It was clarified that the calculations of deprotonation energy and hydroxyl stretching frequency were strongly dependent on the lattice configuration surrounding the Si(OH)AI acid center, therefore, it was obscure using these properties to characterize the acidities from site to site. Nevertheless, adsorption energy of probe molecule on zeolite cluster with adequate size would reflect practically the acid strength corresponding to different zeolite structures. (c) 2005 Elsevier B.V. All rights reserved.
关键词[WOS]: DENSITY-FUNCTIONAL THEORY ;  BRIDGING HYDROXYL-GROUPS ;  AB-INITIO ;  MAS NMR ;  VIBRATIONAL FREQUENCIES ;  INFRARED-SPECTROSCOPY ;  CATALYTIC-PROPERTIES ;  EXTERNAL SURFACE ;  MOLECULAR-SIEVE ;  N-BUTANE
语种: 英语
原文出处: 查看原文
WOS记录号: WOS:000235263100003
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/98031
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.Liaoning Normal Univ, Dept Chem, Inst Chem Functionalized Mat, Dalian 116029, Peoples R China
2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China

Recommended Citation:
Zhou, DH,Bao, Y,Yang, MM,et al. DFT studies on the location and acid strength of Bronsted acid sites in MCM-22 zeolite[J]. JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL,2006,244(1-2):11-19.
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