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Selective Oxidation of Methane to Methanol Catalyzed, with C[BOND]H Activation, by Homogeneous, Cationic Gold

Authors

  • CJ Jones,

    1. University of Southern California, Department of Chemistry, Loker Hydrocarbon Institute, Los Angeles, CA 90089, USA, Fax: (+) 213-821-2656
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  • Doug Taube,

    1. University of Southern California, Department of Chemistry, Loker Hydrocarbon Institute, Los Angeles, CA 90089, USA, Fax: (+) 213-821-2656
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  • Vadim R. Ziatdinov,

    1. University of Southern California, Department of Chemistry, Loker Hydrocarbon Institute, Los Angeles, CA 90089, USA, Fax: (+) 213-821-2656
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  • Roy A. Periana Prof. Dr.,

    1. University of Southern California, Department of Chemistry, Loker Hydrocarbon Institute, Los Angeles, CA 90089, USA, Fax: (+) 213-821-2656
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  • Robert J. Nielsen,

    1. Materials and Process Simulation Center, Beckman Institute (139-74), Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA 91125, USA
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  • Jonas Oxgaard,

    1. Materials and Process Simulation Center, Beckman Institute (139-74), Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA 91125, USA
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  • William A. Goddard III Prof. Dr.

    1. Materials and Process Simulation Center, Beckman Institute (139-74), Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA 91125, USA
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  • This work was supported by NSF Grant CHE-0328121. The computer facilities of the MSC were provided through support from DURIP and MURI. We thank Prof. R. J. Puddephatt for helpful discussion.

Abstract

original image

Kationisches Gold katalysiert die Titelreaktion in stark sauren Lösungsmitteln mit SeVI als stöchiometrischem Oxidans. Bei 180 °C und 27 bar CH4 wurden Katalysatorumsatzzahlen von etwa 30 und Methanolkonzentrationen von etwa 0.6 M mit Selektivitäten >90 % bestimmt. Nach DFT-Rechnungen sind sowohl AuI als auch AuIII geeignete Katalysatoren, die über eine elektrophile C-H-Aktivierung und oxidative Funktionalisierung wirken (siehe Bild).

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