title: Spin-Selective Thermal Activation of Methane by Closed-Shell [TaO3 ](.).
abstract: Thermal reactions of the closed-shell metal-oxide cluster [TaO3 ](+) with methane were investigated by using FTICR mass spectrometry complemented by high-level quantum chemical calculations. While the generation of methanol and formaldehyde is somewhat expected, [TaO3 ](+) remarkably also has the ability to abstract two hydrogen atoms from methane with the elimination of CH2 . Mechanistically, the generation of CH2 O and CH3 OH occurs on the singlet-ground-state surface, while for the liberation of (3) CH2 , a two-state reactivity scenario prevails.
authors.affiliation: Institut für Chemie, Technische Universität Berlin, Straße des 17. Juni 135, 10623, Berlin, Germany.
authors.forename: Shaodong
authors.initials: S
authors.lastname: Zhou
authors.affiliation: Institut für Chemie, Technische Universität Berlin, Straße des 17. Juni 135, 10623, Berlin, Germany.|Institute of Theoretical Chemistry, Jilin University, Changchun, 130023, P.R. China.
authors.forename: Jilai
authors.initials: J
authors.lastname: Li
authors.affiliation: Institut für Chemie, Technische Universität Berlin, Straße des 17. Juni 135, 10623, Berlin, Germany.
authors.forename: Maria
authors.initials: M
authors.lastname: Schlangen
authors.affiliation: Institut für Chemie, Technische Universität Berlin, Straße des 17. Juni 135, 10623, Berlin, Germany. helmut.schwarz@tu-berlin.de.
authors.forename: Helmut
authors.initials: H
authors.lastname: Schwarz
keywords: closed-shell cluster; double hydrogen-atom abstraction; gas-phase reactions; methane activation; quantum chemistry