title: Liberation of three dihydrogens from two ethene molecules as mediated by the tantalum nitride anion cluster Ta3N2-at room temperature.
abstract: The reactivity of gas-phase cluster anions Ta3N2-with C2H4under thermal collision conditions was studied by mass spectrometry in conjunction with density functional theory calculations. The full dehydrogenation of the C2H4molecule was observed, with the formation of two dihydrogen molecules. Interestingly, the two carbon atoms originating from the first C2H4molecule are used to construct another cluster Ta3N2C2-, which can activate one more C2H4releasing one H2molecule. Therefore, three dihydrogen molecules are liberated from two ethene molecules in the overall reaction. The full dehydrogenation of C2H4by gas-phase anions as well as the structure and reactivity of M-N-C (M: transition metal) cluster is reported for the first time. The properties of Ta3N2-and Ta3N2C2-elucidated herein are of use in providing fundamental information that is necessary to tailor the design of new and effective catalysts by applying the related materials.
authors.affiliation: The Institute for Chemical Physics, Key Laboratory of Cluster Science, School of Chemistry, Beijing Institute of Technology, 100081, Beijing, People's Republic of China. majiabi@bit.edu.cn.
authors.forename: Ji-Chuang
authors.initials: JC
authors.lastname: Hu
authors.affiliation: The Institute for Chemical Physics, Key Laboratory of Cluster Science, School of Chemistry, Beijing Institute of Technology, 100081, Beijing, People's Republic of China. majiabi@bit.edu.cn.
authors.forename: Lin-Lin
authors.initials: LL
authors.lastname: Xu
authors.affiliation: State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, 100190, Beijing, People's Republic of China.
authors.forename: Hai-Fang
authors.initials: HF
authors.lastname: Li
authors.affiliation: Institute for Optics and Atomic Physics, Technische Universität Berlin, 10623 Berlin, Germany. fielicke@physik.tu-berlin.de.
authors.forename: David Yubero
authors.initials: DY
authors.lastname: Valdivielso
authors.affiliation: Institute for Optics and Atomic Physics, Technische Universität Berlin, 10623 Berlin, Germany. fielicke@physik.tu-berlin.de.
authors.forename: André
authors.initials: A
authors.lastname: Fielicke
authors.affiliation: State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, 100190, Beijing, People's Republic of China.
authors.forename: Sheng-Gui
authors.initials: SG
authors.lastname: He
authors.affiliation: The Institute for Chemical Physics, Key Laboratory of Cluster Science, School of Chemistry, Beijing Institute of Technology, 100081, Beijing, People's Republic of China. majiabi@bit.edu.cn.
authors.forename: Jia-Bi
authors.initials: JB
authors.lastname: Ma