Hydrogen-atom abstraction from methane by stoichiometric vanadium-silicon heteronuclear oxide cluster cations
文献类型：期刊论文
| 作者 | Ding, Xun-Lei1; Zhao, Yan-Xia1,2; Wu, Xiao-Nan1,2; Wang, Zhe-Chen1,2; Ma, Jia-Bi1,2; He, Sheng-Gui1 |
| 刊名 | Chemistry-a european journal
 |
| 出版日期 | 2010 |
| 卷号 | 16期号:37页码:11463-11470 |
| 关键词 | C-h activation Cluster compounds Density functional calculations Mass spectrometry Methane activation Radicals |
| ISSN号 | 0947-6539 |
| DOI | 10.1002/chem.201001297 |
| 通讯作者 | He, sheng-gui(shengguihe@iccas.ac.cn) |
| 英文摘要 | Vanadium-silicon heteronuclear oxide cluster cations were prepared by laser ablation of a v/si mixed sample in an o-2 background. reactions of the heteronuclear oxide cations with methane in a fast-flow reactor were studied with a time-of-flight (tof) mass spectrometer to detect the cluster distribution before and after the reactions. hydrogen abstraction reactions were identified over stoichiometric cluster cations [(v2o5)(n)(sio2)(m)](+) (n = 1, m=1-4; n=2, m=1), and the estimated first-order rate constants for the reactions were close to that of the homonuclear oxide cluster v4o10+ with methane. density functional calculations were performed to study the structural, bonding, electronic, and reactivity properties of these stoichiometric oxide clusters. terminal-oxygen-centered radicals (o-t(center dot)) were found in all of the stable isomers. these o-t(center dot) radicals are active sites of the clusters in reaction with ch4 center dot the o-t(center dot) radicals in [v2o5(sio2)(1-4)](+) clusters are bonded with si rather than v atoms. all the hydrogen abstraction reactions are favorable both thermodynamically and kinetically. this work reveals the unique properties of metal/nonmetal heteronuclear oxide clusters, and may provide new insights into ch4 activation on silica-supported vanadium oxide catalysts. |
| WOS关键词 | GAS-PHASE REACTIVITY ; SELECTIVE OXIDATION ; METAL-IONS ; VIBRATIONAL SPECTROSCOPY ; HETEROGENEOUS CATALYSIS ; ELECTRONIC-STRUCTURE ; BOND ACTIVATION ; DENSITY ; FORMALDEHYDE ; OXYGEN |
| WOS研究方向 | Chemistry |
| WOS类目 | Chemistry, Multidisciplinary |
| 语种 | 英语 |
| WOS记录号 | WOS:000283386600030 |
| 出版者 | WILEY-V C H VERLAG GMBH |
| URI标识 | http://www.irgrid.ac.cn/handle/1471x/2414492 |
| 专题 | 中国科学院大学 |
| 通讯作者 | He, Sheng-Gui |
| 作者单位 | 1.Chinese Acad Sci, State Key Lab Struct Chem Unstable & Stable Speci, Beijing Natl Lab Mol Sci, Inst Chem, Beijing 100190, Peoples R China 2.Chinese Acad Sci, Grad Sch, Beijing 100039, Peoples R China |
| 推荐引用方式 GB/T 7714 | Ding, Xun-Lei,Zhao, Yan-Xia,Wu, Xiao-Nan,et al. Hydrogen-atom abstraction from methane by stoichiometric vanadium-silicon heteronuclear oxide cluster cations[J]. Chemistry-a european journal,2010,16(37):11463-11470. |
| APA | Ding, Xun-Lei,Zhao, Yan-Xia,Wu, Xiao-Nan,Wang, Zhe-Chen,Ma, Jia-Bi,&He, Sheng-Gui.(2010).Hydrogen-atom abstraction from methane by stoichiometric vanadium-silicon heteronuclear oxide cluster cations.Chemistry-a european journal,16(37),11463-11470. |
| MLA | Ding, Xun-Lei,et al."Hydrogen-atom abstraction from methane by stoichiometric vanadium-silicon heteronuclear oxide cluster cations".Chemistry-a european journal 16.37(2010):11463-11470. |
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来源：中国科学院大学
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