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题名: Stability and reactivity of active sites for direct benzene oxidation to phenol in Fe/ZSM-5: A comprehensive periodic DFT study
作者: Li, Guanna1, 3;  Pidko, Evgeny A.2;  van Santen, Rutger A.2;  Feng, Zhaochi1;  Li, Can1;  Hensen, Emiel J. M.2
关键词: Direct benzene oxidation ;  Fe/ZSM-5 ;  Reaction mechanism ;  DFT calculations ;  Binuclear sites ;  N2O dissociation ;  Phenolate
刊名: JOURNAL OF CATALYSIS
发表日期: 2011-12-01
DOI: 10.1016/j.jcat.2011.07.008
卷: 284, 期:2, 页:194-206
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences ;  Technology
类目[WOS]: Chemistry, Physical ;  Engineering, Chemical
研究领域[WOS]: Chemistry ;  Engineering
英文摘要: The stability of isolated extraframework Fe2+ ions in ZSM-5 zeolite and their reactivity in the benzene to phenol oxidation were studied by periodic OFT calculations. Mononuclear iron(II) cations can only be stabilized at very specific exchange sites of ZSM-5 zeolite. Accordingly, iron will be predominantly present as oxygenated/hydroxylated mono- and binuclear iron complexes in Fe/ZSM-5. The reactivity of isolated Fe2+. does not depend on the local coordination environment around iron, whereas the steric constraints imposed by the zeolite lattice are important for the overall catalytic reactivity. [FeO](+), [HOFe(mu-O)FeOH](2+), [Fe(mu-O)(2)Fe](2+), [Fe(mu-O)Fe](2+). extraframework complexes are also potential sites for benzene activation. The reaction is however not catalytic in these cases because the vacant active site cannot be regenerated. The presence of basic extraframework O ligands in these complexes favors phenol dissociation resulting in the formation of stable grafted phenolate species, and ultimately, to the deactivation of the oxygenated iron complexes. (C) 2011 Elsevier Inc. All rights reserved.
关键词[WOS]: NITROUS-OXIDE DECOMPOSITION ;  DENSITY-FUNCTIONAL THEORY ;  OVER-EXCHANGED FE/ZSM5 ;  MOLECULAR-DYNAMICS SIMULATION ;  SELECTIVE CATALYTIC-REDUCTION ;  TOTAL-ENERGY CALCULATIONS ;  EXTRA-FRAMEWORK GALLIUM ;  BINUCLEAR FE COMPLEXES ;  AUGMENTED-WAVE METHOD ;  BRIDGED IRON SITES
语种: 英语
WOS记录号: WOS:000298527000009
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/142583
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, Peoples R China
2.Eindhoven Univ Technol, Schuit Inst Catalysis, Inorgan Mat Chem Grp, NL-5600 MB Eindhoven, Netherlands
3.Chinese Acad Sci, Grad Univ, Beijing 100049, Peoples R China

Recommended Citation:
Li, Guanna,Pidko, Evgeny A.,van Santen, Rutger A.,et al. Stability and reactivity of active sites for direct benzene oxidation to phenol in Fe/ZSM-5: A comprehensive periodic DFT study[J]. JOURNAL OF CATALYSIS,2011,284(2):194-206.
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