The Catalytic, Selective Partial Oxidation of Alkanes by Transition Metals that Activate Carbon-Hydrigen Bonds

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Lawrence Kool 9310198 This is an attempt to develop a method to convert alkanes directly to partially oxidized products using a platinum catalyst and an aqueous transition-metal oxidant. The approach differs from currently available methods in that it does not require molecular oxygen. This effort includes a critical evaluation of the platinum/aqueous ferric system covering experimental variables, selectivity at high conversion, and elucidation of the mechanism, which is thought to involve an alkylplatinum hydride intermediate; catalyst support effects; substitution of palladium for platinum; the use of various aqueous transition-metal oxidants; and the design, synthesis, and evaluation of soluble organoplatinum complexes that may model the carbon-hydrogen bond cleavage on the platinum surface. Direct partial oxidation of light alkanes (methane, propane, natural gas, etc.) is an important objective of catalytic technology; current methods are either very limited in scope or are cumbersome multistep processes. The products of such processes, such as methanol, ethanol, formaldehyde, acetic acid, etc., have many uses as chemical feedstocks, fuels, or monomers, or they can be further processed to improve existing fuels. Although there is much work toward this objective, the approach in this work is a radical departure from conventional efforts. This is a collaboration with A. E. Shilov at the Institute of Chemical Physics in Chernogolovka, Russia.