CH Activation and Oxidation of Methane to Methanol in High Yield with Novel Pt Complexes

April 27, 1999 - 12:00pm
Bldg. 90
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Methane is greatly underutilized material in spite of it being an ideal fuel, chemical reductant and material precursor for industrialized nations because of the low cost, ready availability and low CO2 generation potential.  This poor utilization can be traced to the lack of catalysts that allow methane to efficiently react under typical reaction conditions. We report on novel, molecular, non-free radical, catalysts will be discussed that allows the direct, low temperature, oxidative conversion of methane to a methanol equivalent product in 70% one-pass yield. A particularly effective system is based on 20mM solutions of (bipyrimidine)PtCl2 in concentrated sulfuric acid.  Reaction of methane at 500 psig and 220oC with this solution result in 90% conversion of methane to methyl bisulfate in 80% selectivity (~70% one-pass yield) based on added methane. The reaction is proposed to proceed via CH activation of methane by Pt(II) species to generate a platinum-methyl intermediate that is oxidized to generate the product, methyl bisulfate.  A platinum-methane complex may be an intermediate before the CH activation step as extensive H exchange between methane and the acid solvent is observe in the presence of the catalyst. Control reactions show that the high selectivity and yield is possible because the methyl bisulfate is at least 10 - 100 times less reactive than methane.  Other applications of molecular, CH Activation-based, Oxidation catalysts will be discussed.

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