Possible active sites in Fe/ZSM-5 zeolite for the direct benzene hydroxylation to phenol: 1. mu-Oxo[Fe, M] species (M = Fe, Al)
文献类型：期刊论文
| 作者 | Yang, Gang; Zhou, Danhong; Liu, Xianchun; Han, Xiuwen; Bao, Xinhe |
| 刊名 | journal of molecular structure
 |
| 出版日期 | 2006-09-18 |
| 卷号 | 797期号:1-3页码:131-139 |
| 关键词 | ZSM-5 zeolite benzene hydroxylation density functional alpha-oxygen |
| 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. |
| WOS标题词 | science & technology ; physical sciences |
| 类目[WOS] | chemistry, physical |
| 研究领域[WOS] | chemistry |
| 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 |
| 收录类别 | SCI |
| 语种 | 英语 |
| WOS记录号 | WOS:000241544100016 |
| 公开日期 | 2015-11-17 |
| 源URL | [http://159.226.238.44/handle/321008/139941]  |
| 专题 | 大连化学物理研究所_中国科学院大连化学物理研究所 |
| 作者单位 | Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China |
| 推荐引用方式 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. |
入库方式： OAI收割
来源：大连化学物理研究所
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