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题名: The formation mechanism of Mo-methylidene species over Mo/HBeta catalysts for heterogeneous olefin metathesis: A density functional theory study
作者: Guan, Jing1;  Yang, Gang1;  Zhou, Danhong1, 2;  Zhang, Weiping1;  Liu, Xianchun1;  Han, Xiuwen1;  Bao, Xinhe1
通讯作者: 包信和
关键词: Active sites ;  Density functional calculations ;  Mo/HBeta catalysts ;  Olefin metathesis ;  Oxidation states
刊名: JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL
发表日期: 2009-03-02
DOI: 10.1016/j.molcata.2008.10.044
卷: 300, 期:1-2, 页:41-47
收录类别: SCI
文章类型: Article
部门归属: 5
项目归属: 502
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: Density Functional Theory (DFT) calculations were performed to optimize the Mo active sites in HBeta zeolite catalysts as well as to locate the reaction pathways to form the Mo-methylidene species. Two different Mo active sites. i.e., the oxidized (MoO2)-O-VI and its reduced form (MoO)-O-V(OH), were developed and incorporated into HBeta zeolites by replacing a pair of Bronsted acidic sites. The Mo-methylidene species were found to be produced through two elementary reaction steps, and the Mo-oxametallacyclobutanes were identified as the intermediates. The activation barriers of the decompositions of the oxametallacyclobutane intermediates (Step 2) were estimated to be higher than those of the ethene addition on the Mo active sites (Step 1). The oxidation states of the Mo centers exerted marked influences on the stabilities of the intermediates as well as oil the activation barriers and reaction heats of Steps 1 and 2, which were elucidated by the electronic properties of the O-b-ligands directly bonded to the Mo centers. Both free energy barriers and reaction heats have indicated that the whole processes of generating the Mo-methylidene species were preferred over the Mo(VI) rather than Mo(V) active site. Accordingly. the Mo(VI) active site was more efficient in catalyzing the formation of Mo-methylidene species in the heterogeneous Mo/HBeta catalytic systems. (C) 2008 Elsevier B.V. All rights reserved.
关键词[WOS]: PHOTOREDUCED SILICA-MOLYBDENA ;  X-RAY-ABSORPTION ;  ALUMINA CATALYSTS ;  ZEOLITE-BETA ;  ACID SITES ;  CHEMISORBED CYCLOPROPANE ;  COORDINATION-NUMBER ;  CARBENE COMPLEXES ;  DFT CALCULATIONS ;  OXO BONDS
语种: 英语
原文出处: 查看原文
WOS记录号: WOS:000264013400007
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/102263
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
2.Liaoning Normal Univ, Coll Chem & Chem Engn, Inst Chem Functionalized Mat, Dalian 116029, Peoples R China

Recommended Citation:
Guan, Jing,Yang, Gang,Zhou, Danhong,et al. The formation mechanism of Mo-methylidene species over Mo/HBeta catalysts for heterogeneous olefin metathesis: A density functional theory study[J]. JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL,2009,300(1-2):41-47.
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