Spin‐Selective Thermal Activation of Methane by Closed‐Shell [TaO3]+ |
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| Authors: | Dr Shaodong Zhou Dr Jilai Li Dr Maria Schlangen Prof?Dr Helmut Schwarz |
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| Affiliation: | 1. Institut für Chemie, Technische Universit?t Berlin, Berlin, Germany;2. Institute of Theoretical Chemistry, Jilin University, Changchun, P.R. China |
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| 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 CH2O and CH3OH occurs on the singlet‐ground‐state surface, while for the liberation of 3CH2, a two‐state reactivity scenario prevails. |
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| Keywords: | closed-shell cluster double hydrogen-atom abstraction gas-phase reactions methane activation quantum chemistry |
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