Stability and reactivity of active sites for direct benzene oxidation to phenol in Fe/ZSM-5: A comprehensive periodic DFT study
文献类型：期刊论文
| 作者 | Li, Guanna1,3; Pidko, Evgeny A.2; van Santen, Rutger A.2; Feng, Zhaochi1; Li, Can1; Hensen, Emiel J. M.2 |
| 刊名 | journal of catalysis
 |
| 出版日期 | 2011-12-01 |
| 卷号 | 284期号:2页码:194-206 |
| 关键词 | Direct benzene oxidation Fe/ZSM-5 Reaction mechanism DFT calculations Binuclear sites N2O dissociation Phenolate |
| 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. |
| WOS标题词 | science & technology ; physical sciences ; technology |
| 类目[WOS] | chemistry, physical ; engineering, chemical |
| 研究领域[WOS] | chemistry ; engineering |
| 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 |
| 收录类别 | SCI |
| 语种 | 英语 |
| WOS记录号 | WOS:000298527000009 |
| 公开日期 | 2015-11-17 |
| 源URL | [http://159.226.238.44/handle/321008/142583]  |
| 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 | 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 |
| 推荐引用方式 GB/T 7714 | 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. |
| APA | Li, Guanna,Pidko, Evgeny A.,van Santen, Rutger A.,Feng, Zhaochi,Li, Can,&Hensen, Emiel J. M..(2011).Stability and reactivity of active sites for direct benzene oxidation to phenol in Fe/ZSM-5: A comprehensive periodic DFT study.journal of catalysis,284(2),194-206. |
| MLA | Li, Guanna,et al."Stability and reactivity of active sites for direct benzene oxidation to phenol in Fe/ZSM-5: A comprehensive periodic DFT study".journal of catalysis 284.2(2011):194-206. |
入库方式： OAI收割
来源：大连化学物理研究所
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