In situ studies of the Mars van Krevelen mechanism in hydrocarbon oxidation.
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Metal oxide-catalyzed selective oxidations follow the Mars van Krevelen mechanism. The organic reactant is oxidized by lattice oxide ions at the surface; these are replenished by dioxygen dissociation with surface and solid state diffusion to reoxidize surface sites. Studies using a flow microbalance reactor to examine butane oxidation by vanadyl pyrophosphate catalysts have determined the kinetics of catalyst reduction and reoxidation in the Mars van Krevelen scheme. Oxygen removal from the lattice is too slow to account for the overall reaction rate. The Mars van Krevelen mechanism using catalyst lattice oxygen can account for only about 5% of the total oxidation activity. VPO catalysts for butane oxidation and Bi-Mo oxide catalysts for propylene oxidation use lattice oxygen to much different extents, providing useful tests of microbalance-based mechanistic studies. This is an abstract of a paper presented at the 228th ACS National Meeting (Philadelphia, PA 8/22-26/2004).