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Diatomic [CuO]+ and Its Role in the Spin-Selective Hydrogen- and Oxygen-Atom Transfers in the Thermal Activation of Methane

Authors

  • Dipl.-Chem. Nicolas Dietl,

    1. Institut für Chemie, Technische Universität Berlin, Strasse des 17. Juni 135, 10623 Berlin (Germany), Fax: (+49) 30-314-21102
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  • Dipl.-Chem. Christian van der Linde,

    1. Institut für Physikalische Chemie, Christian-Albrechts-Universität zu Kiel, Olshausenstrasse 40, 24098 Kiel (Germany)
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  • Dr. Maria Schlangen,

    1. Institut für Chemie, Technische Universität Berlin, Strasse des 17. Juni 135, 10623 Berlin (Germany), Fax: (+49) 30-314-21102
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  • Prof. Dr. Martin K. Beyer,

    1. Institut für Physikalische Chemie, Christian-Albrechts-Universität zu Kiel, Olshausenstrasse 40, 24098 Kiel (Germany)
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  • Prof. Dr. Helmut Schwarz

    Corresponding author
    1. Institut für Chemie, Technische Universität Berlin, Strasse des 17. Juni 135, 10623 Berlin (Germany), Fax: (+49) 30-314-21102
    • Institut für Chemie, Technische Universität Berlin, Strasse des 17. Juni 135, 10623 Berlin (Germany), Fax: (+49) 30-314-21102
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  • Financial support by the Fonds der Chemischen Industrie and the Deutsche Forschungsgemeinschaft, in particular the Cluster of Excellence “Unifying Concepts in Catalysis” (coordinated by the Technische Universität Berlin and funded by the DFG) is acknowledged. We thank the Institut für Mathematik at the Technische Universität Berlin for computational resources and appreciate insightful discussions with Robert Berger, Max Holthausen, Chen Hui, Martin Lerch, Sason Shaik, and Xinhao Zhang.

Abstract

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The final piece in an intriguing puzzle: More than ten years after its theoretical prediction to serve as a powerful converter of methane to methanol, the bare [CuO]+ cation has been successfully generated in the gas phase. A combination of mass spectrometry and DFT calculations revealed the crucial role of two-state reactivity and oxygen-centered radicals in the selectivity in the oxidation of methane.

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