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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

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Cationic gold catalyzes the title reaction in strong acid solvents with SeVI as the stoichiometric oxidant. At 180 oC and 27 bar of CH4 turnover numbers of about 30 and methanol concentrations of 0.6 M have been observed with selectivities >90%. DFT calculations indicate that cationic AuI and AuIII are both viable catalysts that operate by electrophilic C[BOND]H activation and oxidative functionalization (see picture).

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