Abstract
Reactions of CO with H 2O over supported rhodium to form H 2, CH 4, and CO 2 were studied. The formation of methane appears to occur via the water gas shift reaction, followed by the hydrogenation of surface carbon. By operating at sufficiently small contact times it was possible to follow only the water gas shift reaction. The turnover frequency for this reaction was a function of the type of support, resulting in the turnover frequency sequence: Rh Al 2O 3 > Rh Y zeolite > Rh SiO 2 > RhNaY zeolite. This sequence correlates with the activity of supported rhodium in the formation of surface carbon. On the basis of this relationship and kinetic data it appears that surface carbon is an important intermediate in the water gas shift reaction. By contrast, a previous study indicated that over supported ruthenium the principal reaction mechanism involved molecular rather than dissociated CO. The turnover frequencies observed with supported Rh were more than an order of magnitude less than those observed with supported Ru.
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