Studies on self-sustained reaction-rate oscillations. II. The role of carbon and oxides in the oscillatory oxidation of carbon monoxide on platinum

V. A. Burrows, S. Sundaresan, Y. J. Chabal, S. B. Christman

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Abstract

CO oxidation on a platinum foil was studied in a high pressure flow cell (102-102 Pa) and an UHV chamber (10-8 -5 × 104 Pa) both interfaced to a surface infrared spectrometer. Real-time surface infrared and calorimetry experiments performed in the cell during oscillatory oxidation indicated a slow periodic variation (∼ 40%) in the number of active sites, the period of which was commensurate with that of the reaction-rate oscillations. Auger spectroscopy performed in the UHV chamber showed that surface carbon quantitatively accounted for the surface deactivation, as evidenced by the inverse correlation of the number of surface sites active towards CO adsorption with the surface carbon concentration and by the demonstration that, at the oscillation temperatures, carbon can diffuse from the bulk to the surface, oxygen can remove surface carbon and adsorbed CO can block carbon diffusion. Although silicon oxide was always detected on the surface with infrared spectroscopy, no periodic variation in it could be observed during the reaction-rate oscillations. Auger studies confirmed that the maximum and the variations in surface concentration of silicon oxide could not account for the variations in the number of active sites. A mechanism is therefore proposed in which carbon is driving the long-period self-sustained oscillations in the rate of CO oxidation on Pt.

Original languageEnglish (US)
Pages (from-to)110-135
Number of pages26
JournalSurface Science
Volume180
Issue number1
DOIs
StatePublished - Feb 1 1987

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ASJC Scopus subject areas

  • Condensed Matter Physics
  • Surfaces and Interfaces
  • Surfaces, Coatings and Films
  • Materials Chemistry

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