title: Activation and Transformation of Ethane by Au2 VO3(+) Clusters with Closed-Shell Electronic Structures.
abstract: The study of chemical reactions between gold-containing heteronuclear oxide clusters and small molecules can provide molecular level mechanisms to understand the excellent activity of gold supported by metal oxides. While the promotion role of gold in alkane transformation was identified in the clusters with atomic oxygen radicals (O(-.)), the role of gold in the systems without O(-.) is not clear. By employing mass spectrometry and quantum chemistry calculations, the reactivity of Au2 VO3(+) clusters with closed-shell electronic structures toward ethane was explored. Both the dehydrogenation and ethene elimination channels were identified. It is gold rather than oxygen species initiating the C-H activation. The Au-Au dimer formed during the reactions plays important roles in ethane transformation. The reactivity comparison between Au2 VO3(+) and bare Au2(+) demonstrates that Au2 VO3(+) not only retains the property of bare Au2(+) that transforming ethane to dihydrogen, but also exhibits new functions in converting ethane to ethene, which reveals the importance of the composite system. This study provides a further understanding of the reactivity of metal oxide supported gold in alkane activation and transformation.
authors.affiliation: Beijing National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, P. R. China.|University of Chinese Academy of Sciences, Beijing, 100049, P. R. China.
authors.forename: Ya-Ke
authors.initials: YK
authors.lastname: Li
authors.affiliation: Beijing National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, P. R. China.|University of Chinese Academy of Sciences, Beijing, 100049, P. R. China.
authors.forename: Zi-Yu
authors.initials: ZY
authors.lastname: Li
authors.affiliation: Beijing National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, P. R. China. chemzyx@iccas.ac.cn.
authors.forename: Yan-Xia
authors.initials: YX
authors.lastname: Zhao
authors.affiliation: Beijing National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, P. R. China.|University of Chinese Academy of Sciences, Beijing, 100049, P. R. China.
authors.forename: Qing-Yu
authors.initials: QY
authors.lastname: Liu
authors.affiliation: Beijing National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, P. R. China.|University of Chinese Academy of Sciences, Beijing, 100049, P. R. China.
authors.forename: Jing-Heng
authors.initials: JH
authors.lastname: Meng
authors.affiliation: Beijing National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, P. R. China. shengguihe@iccas.ac.cn.
authors.forename: Sheng-Gui
authors.initials: SG
authors.lastname: He
keywords: C−H activation; density functional theory; ethene; gold; mass spectrometry; vanadium