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题名: Possible active sites in Fe/ZSM-5 zeolite for the direct benzene hydroxylation to phenol: 1. mu-Oxo[Fe, M] species (M = Fe, Al)
作者: Yang, Gang;  Zhou, Danhong;  Liu, Xianchun;  Han, Xiuwen;  Bao, Xinhe
关键词: ZSM-5 zeolite ;  benzene hydroxylation ;  density functional ;  alpha-oxygen
刊名: JOURNAL OF MOLECULAR STRUCTURE
发表日期: 2006-09-18
DOI: 10.1016/j.molstruc.2006.03.059
卷: 797, 期:1-3, 页:131-139
收录类别: SCI
文章类型: Article
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 employed to obtain the configurations of oxo-bridged [Fe, M] exchanged ZSM-5 zeolite clusters, possible active sites for direct benzene hydroxylation. For oxo-bridged [Fe, Fe] species, the Fe-Fe and Fe-O distances in Configurations a, b, c, d, e(1) and f were more consistent with experimental (ca. 2.53 or 3.06 angstrom) than in the cluster models designed by Yakovlev et at. with two framework Al atoms nearby. For oxo-bridged [Fe,M] species, the geometric parameters of Configurations g, i and j agreed well with experimental. Configuration i was found to be of higher stability by 64.2 kJ mol(-1) compared to its isomer Configuration k(1). +II and +III constituted the dominant valence states for Fe in Fe/ZSM-5 zeolite, and the state of mixed +II and +III valences did exist in ZSM-5 zeolite as in Configuration b(1), b(2) or c. Fe of +I state was absolutely non-existent in ZSM-5 zeolite even if predefined so. The calculated reaction heats of "alpha-oxygen" formation clearly showed that the oxidation processes were always facilitated by N2O than O-2. The reaction heats of ZSM-5 zeolites exchanged with mono-Fe and binuclear Fe species (n -> o, a(1,2) -> b(1,2) and e(1) -> f) were -114.9, -65.3, -67.4 and -48.8 kJ mol(-1), respectively, in excellent agreement with the results obtained by Ryder, Yakovlev et al. Moreover, "alpha-oxygen" generation was favored by introduction of extra-framework Al (i -> j: -73.9 kJ mol(-1)) compared to the binuclear Fe species. All factors considered, the best candidates for "alpha-oxygen" generation were Configuration al, 2 for oxo-bridged [Fe,Fe] species and Configuration i for oxo-bridged [Fe,Al] species, respectively. (c) 2006 Published by Elsevier B.V.
关键词[WOS]: X-RAY-ABSORPTION ;  DENSITY-FUNCTIONAL THEORY ;  OVER-EXCHANGED FE/ZSM5 ;  SELECTIVE OXIDATION ;  NITROUS-OXIDE ;  N2O DECOMPOSITION ;  ALPHA-OXYGEN ;  ONIOM METHOD ;  FE-ZSM-5 ;  ACTIVATION
语种: 英语
WOS记录号: WOS:000241544100016
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/139941
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:
Yang, Gang,Zhou, Danhong,Liu, Xianchun,et al. Possible active sites in Fe/ZSM-5 zeolite for the direct benzene hydroxylation to phenol: 1. mu-Oxo[Fe, M] species (M = Fe, Al)[J]. JOURNAL OF MOLECULAR STRUCTURE,2006,797(1-3):131-139.
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