NONLINEAR EFFECTS IN ADSORPTION AND REACTION DYNAMICS AT SURFACES: KINETIC OSCILLATIONS UNDER SCRUTINY

David A. King
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David A. King: Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, UK

Surface Review and Letters (SRL), 1994, vol. 01, issue 04, 435-442

Abstract: A number of catalytic reactions exhibit complex dynamical behavior, including kinetic oscillations with both temporal and spatial characteristics. Attention has been focused on theCO+ NOandCO+O2reactions on Pt{100}. Recent molecular beam studies conducted at Cambridge on the interaction of CO with Pt{100} have provided the basis for a new mechanism for oscillatory behavior. The rate of growth of(1×1)islands on the quasihexagonal reconstructed phase of Pt{100} isstrongly nonlinearwith respect to the local CO coverage on the hex-R phase at temperatures between 380 and 410 K, with a reaction order of 4. This strong nonlinearity results in a flux-dependent sticking probability for CO at this temperature, and detailed modeling also reproduces the major features in the oscillatory behavior observed for theCO+NOreaction. An important effect of the nonlinearity in both theCO+NOandCO+O2oscillatory behavior at high temperatures is the maintenance of in-phase behavior across the surface during oscillations.

Date: 1994
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DOI: 10.1142/S0218625X94000400

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