Reactivity of Oxygen Radical Anions Bound to Scandia Nanoparticles in the Gas Phase: C-H Bond Activation
文献类型：期刊论文
| 作者 | Tian, Li-Hua1,2; Meng, Jing-Heng1,3; Wu, Xiao-Nan1; Zhao, Yan-Xia1; Ding, Xun-Lei1; He, Sheng-Gui1; Ma, Tong-Mei2 |
| 刊名 | CHEMISTRY-A EUROPEAN JOURNAL
 |
| 出版日期 | 2014-01-20 |
| 卷号 | 20期号:4页码:1167-1175 |
| 关键词 | Ch Activation Cluster Compounds Mass Spectrometry Radical Ions Scandium |
| ISSN号 | 0947-6539 |
| DOI | 10.1002/chem.201302705 |
| 英文摘要 | The activation of CH bonds in alkanes is currently a hot research topic in chemistry. The atomic oxygen radical anion (O-.) is an important species in CH activation. The mechanistic details of CH activation by O-. radicals can be well understood by studying the reactions between O-. containing transition metal oxide clusters and alkanes. Here the reactivity of scandium oxide cluster anions toward n-butane was studied by using a high-resolution time-of-flight mass spectrometer coupled with a fast flow reactor. Hydrogen atom abstraction (HAA) from n-butane by (Sc2O3)(N)O- (N=1-18) clusters was observed. The reactivity of (Sc2O3)(N)O- (N=1-18) clusters is significantly sizedependent and the highest reactivity was observed for N=4 (Sc8O13-) and 12 (Sc24O37-). Larger (Sc2O3)(N)O- clusters generally have higher reactivity than the smaller ones. Density functional theory calculations were performed to interpret the reactivity of (Sc2O3)(N)O- (N=1-5) clusters, which were found to contain the O-. radicals as the active sites. The local charge environment around the O-. radicals was demonstrated to control the experimentally observed size-dependent reactivity. This work is among the first to report HAA reactivity of cluster anions with dimensions up to nanosize toward alkane molecules. The anionic O-. containing scandium oxide clusters are found to be more reactive than the corresponding cationic ones in the CH bond activation. |
| 语种 | 英语 |
| WOS记录号 | WOS:000329548000033 |
| 出版者 | WILEY-V C H VERLAG GMBH |
| 源URL | [http://ir.iccas.ac.cn/handle/121111/53073]  |
| 专题 | 中国科学院化学研究所 |
| 通讯作者 | Zhao, Yan-Xia |
| 作者单位 | 1.Chinese Acad Sci, Inst Chem, Beijing Natl Lab Mol Sci, State Key Lab Struct Chem Unstable & Stable Speci, Beijing 100864, Peoples R China 2.S China Univ Technol, Sch Chem & Chem Engn, Guangzhou, Guangdong, Peoples R China 3.Univ Chinese Acad Sci, Beijing, Peoples R China |
| 推荐引用方式 GB/T 7714 | Tian, Li-Hua,Meng, Jing-Heng,Wu, Xiao-Nan,et al. Reactivity of Oxygen Radical Anions Bound to Scandia Nanoparticles in the Gas Phase: C-H Bond Activation[J]. CHEMISTRY-A EUROPEAN JOURNAL,2014,20(4):1167-1175. |
| APA | Tian, Li-Hua.,Meng, Jing-Heng.,Wu, Xiao-Nan.,Zhao, Yan-Xia.,Ding, Xun-Lei.,...&Ma, Tong-Mei.(2014).Reactivity of Oxygen Radical Anions Bound to Scandia Nanoparticles in the Gas Phase: C-H Bond Activation.CHEMISTRY-A EUROPEAN JOURNAL,20(4),1167-1175. |
| MLA | Tian, Li-Hua,et al."Reactivity of Oxygen Radical Anions Bound to Scandia Nanoparticles in the Gas Phase: C-H Bond Activation".CHEMISTRY-A EUROPEAN JOURNAL 20.4(2014):1167-1175. |
入库方式： OAI收割
来源：化学研究所
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