ICCAS OpenIR
Hydrogen-Atom Abstraction from Methane by Stoichiometric Vanadium-Silicon Heteronuclear Oxide Cluster Cations
Ding, Xun-Lei1; Zhao, Yan-Xia1,2; Wu, Xiao-Nan1,2; Wang, Zhe-Chen1,2; Ma, Jia-Bi1,2; He, Sheng-Gui1
2010
Source PublicationCHEMISTRY-A EUROPEAN JOURNAL
ISSN0947-6539
Volume16Issue:37Pages:11463-11470
AbstractVanadium-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.
KeywordC-h Activation Cluster Compounds Density Functional Calculations Mass Spectrometry Methane Activation Radicals
DOI10.1002/chem.201001297
Indexed BySCI
Language英语
WOS IDWOS:000283386600030
PublisherWILEY-V C H VERLAG GMBH
Citation statistics
Cited Times:72[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.iccas.ac.cn/handle/121111/70700
Collection中国科学院化学研究所
Corresponding AuthorHe, Sheng-Gui
Affiliation1.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
Recommended Citation
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.
Files in This Item:
There are no files associated with this item.
Related Services
Recommend this item
Bookmark
Usage statistics
Export to Endnote
Google Scholar
Similar articles in Google Scholar
[Ding, Xun-Lei]'s Articles
[Zhao, Yan-Xia]'s Articles
[Wu, Xiao-Nan]'s Articles
Baidu academic
Similar articles in Baidu academic
[Ding, Xun-Lei]'s Articles
[Zhao, Yan-Xia]'s Articles
[Wu, Xiao-Nan]'s Articles
Bing Scholar
Similar articles in Bing Scholar
[Ding, Xun-Lei]'s Articles
[Zhao, Yan-Xia]'s Articles
[Wu, Xiao-Nan]'s Articles
Terms of Use
No data!
Social Bookmark/Share
All comments (0)
No comment.
 

Items in the repository are protected by copyright, with all rights reserved, unless otherwise indicated.