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Title: Catalytic oxidation of carbon monoxide over Rh/SiO/sub 2/. An in situ infrared and kinetic study

Journal Article · · J. Phys. Chem.; (United States)
DOI:https://doi.org/10.1021/j150649a015· OSTI ID:6697840

The oxidation of CO on Rh/SiO/sub 2/ has been studied by using an in situ infrared cell reactor. The catalytic activity for the rate of CO oxidation was shown to decrease in the sequence Rh(0) > Rh(I) > Rh(Iapprox.III). The results of a temperature-programmed-oxidation study show that both linearly adsorbed (2065 cm/sup -1/) and bridge-bonded (1920 cm/sup -1/) CO react with O/sub 2/ at a faster rate than the CO dicarbonyl species (2092, 2033 cm/sup -1/). A higher oxidation state of Rh, presumably Rh(Iapprox.III), which gave rise to an adsorbed CO species absorbing at 2103 cm/sup -1/, was found to be relatively inactive. The results of a temperature-programmed-reduction study show that the adsorbed CO dicarbonyl species can be converted into the linearly adsorbed species by the addition of H/sub 2/ at room temperature. Unlike Ru/SiO/sub 2/ and Pt/SiO/sub 2/, reaction rate hysteresis did not occur. However, in an oxygen-rich reactant gas mixture, some modification of the reaction rate did occur as a result of the formation of Rh(I). This led to a modest catalyst deactivation. Both heat-transfer effects and diffusion-controlled processes occur at high CO conversions. Meaningful kinetic parameters can only be obtained by considering steady-state conversions which are less than 10%.

Research Organization:
Univ. of Rhode Island, Kingston
OSTI ID:
6697840
Journal Information:
J. Phys. Chem.; (United States), Vol. 88:5
Country of Publication:
United States
Language:
English