Abstract
The oxygen insertion pathway over MoO[sub 3] catalysts has been investigated for the partial oxidation of methane to formaldehyde using transient isotopic labeling under steady-state reaction conditions. Catalyst samples preferentially exposing basal (010) and side (100) planes have been characterized using various techniques including scanning electron microscopy with three-dimensional imaging, BET surface area, X-ray diffraction, X-ray photoelectron spectroscopy, and laser Raman spectroscopy. In addition to isotopic labeling studies, these catalysts have also been examined under steady-state reaction conditions to assess the effect of the concentration of gas-phase oxygen. Results of the characterization and reaction studies suggest that the production of HCHO proceeds via utilization of lattice oxygen through the Mo[double bond]O sites. These sites are then preferentially replenished through bulk diffusion of oxygen. The bridging Mo-O-Mo sites, on the other hand, appear to be involved in complete oxidation and are more easily regenerated by gas-phase oxygen. 19 refs., 8 figs., 3 tabs.
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