Methane Activation by Tantalum Carbide Cluster Anions Ta2C4-
文献类型：期刊论文
| 作者 | Li, Hai-Fang1,2; Zhao, Yan-Xia1; Yuan, Zhen1; Liu, Qing-Yu1,2; Li, Zi-Yu1; Li, Xiao-Na1; Ning, Chuan-Gang3; He, Sheng-Gui1 |
| 刊名 | JOURNAL OF PHYSICAL CHEMISTRY LETTERS
 |
| 出版日期 | 2017-02-02 |
| 卷号 | 8期号:3页码:605-610 |
| 英文摘要 | Methane activation by transition metals is of fundamental interest and practical importance, as this process is extensively involved in the natural gas conversion to fuels and value-added chemicals. While single-metal centers have been well recognized as active sites for methane activation, the active center composed of two or more metal atoms is rarely addressed and the detailed reaction mechanism remains unclear. Here, by using state-of-the-art time-of-flight mass spectrometry, cryogenic anion photoelectron imaging spectroscopy, and quantum-chemical calculations, the cooperation of the two Ta atoms in a dinuclear carbide cluster Ta2C4- for methane activation has been identified. The C-H bond activation takes place predominantly around one Ta atom in the initial stage of the reaction and the second Ta atom accepts the delivered H atom from the C-H bond cleavage. The well-resolved vibrational spectra of the cryogenically cooled anions agree well with theoretical simulations, allowing the clear characterization of the structure of Ta2C4- cluster. The reactivity comparison between Ta2C4- cluster and the carbon-less analogues (Ta2C3- and Ta2C2-) demonstrated that the cooperative effect of the two metal atoms can be well tuned by the carbon ligands in terms of methane activation and transformation. |
| 语种 | 英语 |
| 源URL | [http://ir.iccas.ac.cn/handle/121111/38078]  |
| 专题 | 化学研究所_分子动态与稳态结构实验室 |
| 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.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 3.Tsinghua Univ, Dept Phys, State Key Lab Low Dimens Quantum Phys, Beijing 100084, Peoples R China |
| 推荐引用方式 GB/T 7714 | Li, Hai-Fang,Zhao, Yan-Xia,Yuan, Zhen,et al. Methane Activation by Tantalum Carbide Cluster Anions Ta2C4-[J]. JOURNAL OF PHYSICAL CHEMISTRY LETTERS,2017,8(3):605-610. |
| APA | Li, Hai-Fang.,Zhao, Yan-Xia.,Yuan, Zhen.,Liu, Qing-Yu.,Li, Zi-Yu.,...&He, Sheng-Gui.(2017).Methane Activation by Tantalum Carbide Cluster Anions Ta2C4-.JOURNAL OF PHYSICAL CHEMISTRY LETTERS,8(3),605-610. |
| MLA | Li, Hai-Fang,et al."Methane Activation by Tantalum Carbide Cluster Anions Ta2C4-".JOURNAL OF PHYSICAL CHEMISTRY LETTERS 8.3(2017):605-610. |
入库方式： OAI收割
来源：化学研究所
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