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  • 1
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 87 (1987), S. 742-749 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Periodic modulations of oxygen pressure or temperature were applied in the catalytic oxidation of CO on a Pt(100) surface under isothermal, low pressure conditions. Transitions from aperiodic autonomous oscillations to regular phase-locked behavior could be observed. Computer simulations using a stochastic cellular automaton model yielded qualitatively similar results. The spatial distribution in both experiment and simulation varies essentially in phase over the whole surface area under the influence of the periodic perturbation, while wave propagation in the autonomous system causes more irregular overall behavior.
    Type of Medium: Electronic Resource
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  • 2
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 85 (1986), S. 5328-5336 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The previously observed phenomena of temporal and spatial self-organization during the catalytic oxidation of CO on a Pt(100) surface were computer simulated by use of the cellular automaton technique. The underlying model is footed on the knowledge about the individual reaction steps (adsorption, desorption, surface structural transformation, etc.), which in turn formed the basis of a previous theoretical treatment in terms of the formulation and solution of a set of coupled differential equations. The present result nicely show the formation and propagation of two-dimensional patterns, and they reproduce qualitatively well all the experimental observations. The development of macroscopic patterns even with an a priori perfectly homogeneous surface is a particularly interesting effect.
    Type of Medium: Electronic Resource
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  • 3
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 90 (1989), S. 510-521 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The rate of catalytic CO oxidation on Pt(100) and (110) surfaces at low pressures (≤10−4 Torr) and under isothermal conditions may exhibit sustained temporal oscillations which are coupled with periodic transformations of the surface structures between reconstructed and nonreconstructed phases, the latter exhibiting higher oxygen sticking coefficients and hence higher reactivity. With Pt(100) the two surface phases exhibit a much larger difference in reactivity (=oxygen sticking coefficient) than with Pt(110), which effect accounts for the qualitative differences in the oscillatory behavior: if two of the control parameters (say pO2, T) are kept fixed, the third (pCO) may be varied with Pt(100) over a fairly wide range without leaving the oscillatory region. Minor (〈1%) fluctuations of the partial pressures associated with the varying reaction rate are hence without any noticeable effect. Coupling between surface reaction and diffusion causes wave propagation of the surface phase transformations and therefore spatial self-organization, as demonstrated by scanning LEED experiments. With Pt(110), on the other hand, the oscillatory region is very narrow. In this case mass transport through the gas phase as caused by the small pressure variations associated with the reaction lead to synchronization between different parts of the surface. Computer simulations with the cellular automaton technique confirm qualitatively the experimental findings and support the conclusions reached.
    Type of Medium: Electronic Resource
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