Center for Enabling New Technologies Through Catalysis
A NSF Center for Chemical Innovation
Oxidative Oligomerization of Methane
Senior Investigators: Prof. Melanie Sanford (U. Mich.), Prof. Jim Mayer (U. Wash.).
Methane (the primary component of natural gas) is highly abundant on earth, and will be an increasingly important source of global energy as petroleum supplies are depleted. However, the widespread use of methane remains limited by the difficulty and expense associated with transporting this flammable gas over long distances. As a result, efficient chemical reactions that directly convert methane into more readily transportable higher alkanes would be of great significance for helping to meet growing global energy demands. The goal of this project is to develop transition metal catalysts for the direct oxidative dimerization and/or oligomerization of methane to form higher alkanes using dioxygen as a terminal oxidant. This approach would be highly advantageous, as the current route from methane to higher alkanes requires an energy-intensive sequence involving initial steam reforming to generate syngas followed by Fisher Tropsch synthesis to form the desired hydrocarbon products.
In addition to applications in
methane chemistry, we anticipate that catalysts
developed in this CENTC project will prove
useful for direct oxidative C–C bond-forming
reactions of more complex molecules. The
construction of aryl–aryl, alkyl–aryl, and
alkyl–alkyl bonds is of critical importance in
the synthesis of polymeric materials,
pharmaceuticals, and specialty chemicals. A
route to achieve such C–C bond-forming reactions
selectively starting directly from C–H
substrates would be particularly efficient and
Lanci, M. P.; Remy, M. S.; Lao, D. B.; Sanford, M. S.; Mayer, J. M. “Modulating Sterics in Trimethylplatinum(IV) Diimine Complexes To Achieve C-C Bond-Forming Reductive Elimination”, Organometallics, 2011, 30, 3704-3707.
Remy, M. S.; Cundari, T. R.; Sanford, M. S., "Computational and Experimental Studies of Methyl Group Exchange between Palladium(II) Centers", Organometallics, 2010, 29, 1522-1525.
Lanci, M. P.; Remy, M. S.; Kaminsky, W.; Mayer, J. M.; Sanford, M. S., "Oxidatively Induced Reductive Elimination from (tBu2bpy)Pd(Me)2: Palladium(IV) Intermediates in a One Electron Oxidation Reaction", J. Am. Chem. Soc., 2009, 131, 15618-15620.
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