Mechanistic Studies of C-H Activation Catalysts for Direct Organic Fuel Cell Applications

The goal of this program is to obtain fundamental understanding that will lead to design of catalysts or catalyst systems for C-H bond activation that can function in direct organic fuel cells, and that are based upon molecular species, rather than metal surfaces. In studying C-H activation by platinum complexes, we have used the results of prior mechanistic studies to design complexes that effect C-H activation under milder conditions, and are working on incorporating these concepts into systems for catalytic alkane oxidation. In the area of metal oxo complexes, we have discovered a complex that efficiently oxidizes alcohols at significantly lower reduction potentials than previously observed, apparently by avoiding a undesirable high energy one-electron mechanism. Our investigations are directed at extending this discovery to the design of catalysts that can operate at fuel-cell-relevant potentials.