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Possible active sites in Fe/ZSM-5 zeolite for the direct benzene hydroxylation to phenol: 1. mu-Oxo[Fe, M] species (M = Fe, Al)
Yang, Gang; Zhou, Danhong; Liu, Xianchun; Han, Xiuwen; Bao, Xinhe
KeywordZsm-5 Zeolite Benzene Hydroxylation Density Functional Alpha-oxygen
Source PublicationJOURNAL OF MOLECULAR STRUCTURE
2006-09-18
DOI10.1016/j.molstruc.2006.03.059
Volume797Issue:1-3Pages:131-139
Indexed BySCI
SubtypeArticle
WOS HeadingsScience & Technology ; Physical Sciences
WOS SubjectChemistry, Physical
WOS Research AreaChemistry
WOS KeywordX-RAY-ABSORPTION ; DENSITY-FUNCTIONAL THEORY ; OVER-EXCHANGED FE/ZSM5 ; SELECTIVE OXIDATION ; NITROUS-OXIDE ; N2O DECOMPOSITION ; ALPHA-OXYGEN ; ONIOM METHOD ; FE-ZSM-5 ; ACTIVATION
AbstractDensity 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.
Language英语
WOS IDWOS:000241544100016
Citation statistics
Cited Times:19[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/139941
Collection中国科学院大连化学物理研究所
AffiliationChinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
Recommended Citation
GB/T 7714
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.
APA Yang, Gang,Zhou, Danhong,Liu, Xianchun,Han, Xiuwen,&Bao, Xinhe.(2006).Possible active sites in Fe/ZSM-5 zeolite for the direct benzene hydroxylation to phenol: 1. mu-Oxo[Fe, M] species (M = Fe, Al).JOURNAL OF MOLECULAR STRUCTURE,797(1-3),131-139.
MLA Yang, Gang,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)".JOURNAL OF MOLECULAR STRUCTURE 797.1-3(2006):131-139.
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