Yong Yang1, Rob Disselkamp1, Janos Szanyi2, and Charlie Campbell3. (1) Institute for Interfacial Catalysis, Pacific N.W. National Laboratory, 3335 Q Avenue, Richland, WA 99352, (2) Institute for Interfacial Catalysis, Pacific Northwest National Laboratory, 3335 Q Avenue, Richland, WA 99352, (3) Department of Chemistry, University of Washington, Box 351700, Seattle, WA 98195
A novel apparatus has been developed to enable catalytic reaction mechanisms and kinetic parameters to be determined on supported catalyst samples. Here we investigate the reverse water-gas shift (RWGS) reaction on a Cu/gamma-alumina catalyst. We have performed SSITKA experiments that probe the steady-state, and transient, surface formate/carbonate/carbonyl species. Both the input H2:CO2 ratio and temperature dependence have been explored. Transient experiments employing a 12CO2/13CO2 gas switch has enabled the surface adsorbed identity, number of surface adsorbed species (e.g., approximate coverage), and average rate-coefficient yielding products to be determined. The poly-dispersity in chemical intermediate(s) leading to product formation has been explored by computing the reactivity distribution function (RDF) as part of these experiments.