The dynamics of CO oxidation on Pd, Rh, and Pt studied by high-resolution infrared chemiluminescence spectroscopy

Coulston, George W.; Haller, Gary L.
November 1991
Journal of Chemical Physics;11/1/1991, Vol. 95 Issue 9, p6932
Academic Journal
The dynamics of carbon monoxide oxidation on Pd, Rh, and Pt foils were probed under nearly collision-free conditions using high resolution infrared chemiluminescence. Auger electron spectroscopy was used to verify the absence of impurities on the surfaces. The reactants were supplied to the surface through a free jet nozzle source, while a Fourier transform infrared spectrometer operating at 0.012 cm-1 resolution was used to fully resolve the rotational structure of several vibrational transitions in the product CO2 (22 in the case of Pd). In all cases, the product CO2 is vibrationally excited and the apparent vibrational temperatures are in the same order as the peak reaction rates, i.e., Pd>Pt>Rh. The surface coverage of oxygen on Pd was varied by changing the CO[ATOTHER]@B:[/ATOTHER] O2 ratio and the surface temperature and, in both cases, increasing oxygen coverage causes an increase in vibrational excitation of product CO2. On Pt and Rh, the apparent temperatures of different vibrational modes are similar, while on Pd, those levels involved in Fermi resonances that are traditionally called the symmetric stretch levels are selectively populated. From these results, evidence that the activated complex is bent on Pd relative to Pt and Rh and, in all cases, is aligned more or less along the surface normal is presented.


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