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Mechanisms of spatial self-organization in isothermal kinetic oscillations during the catalytic CO oxidation on Pt single crystal surfaces

J. Chem. Phys. 90, 510 (1989); doi:10.1063/1.456501

Issue Date: 1 January 1989

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M. Eiswirth, P. Möller, K. Wetzl, R. Imbihl, and G. Ertl
Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, D-1000 Berlin 33, Federal Republic of Germany
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. The Journal of Chemical Physics is copyrighted by The American Institute of Physics.
History: Received 14 June 1988; accepted 22 September 1988
Permalink: http://link.aip.org/link/?JCPSA6/90/510/1
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KEYWORDS and PACS

Keywords
PACS
  • 82.65.Jv
    Physical chemistry Surface and interface chemistry Heterogeneous catalysis at surfaces
  • 82.20.Mj
    Physical chemistry Chemical kinetics Nonequilibrium kinetics
  • 82.20.Wt
    Physical chemistry Chemical kinetics Computational modeling; simulation
  • 82.20.Hf
    Physical chemistry Chemical kinetics Mechanisms and product distribution
  • YEAR: 1988-89

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PUBLICATION DATA

ISSN:
0021-9606 (print)   1089-7690 (online)
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AIP is a member of CrossRef AIP

REFERENCES (37)
View in Separate Window/Tab
  1. (a) P. Hugo, Ber. Bunsenges. Phys. Chem. 74, 121 (1970);
    2. (b) H. Beusch, P. Fieguth, and E. Wicke, Chem. Ing. Techn. 44, 445 (1972). [ISI] [ChemPort]
  2. L. F. Razón and R. A. Schmitz, Catal. Rev. Sci. Eng. 28, 89 (1986). [ISI] [ChemPort]
  3. H. U. Onken and E. Wicke, Ber. Bunsenges. Phys. Chem. 90, 976 (1986).
  4. L. F. Razón, S.-M. Chang, and R. A. Schmitz, Chem. Eng. Sci. 41, 1561 (1986).
  5. G. Ertl, P. R. Norton, and J. Rüstig, Phys. Rev. Lett. 49, 177 (1982).
  6. M. P. Cox, G. Ertl, R. Imbihl, and J. Rüstig, Surf. Sci. 134, L517 (1983). [Inspec] [ISI] [ChemPort]
  7. M. P. Cox, G. Ertl, and R. Imbihl, Phys. Rev. Lett. 54, 1725 (1985). [ISI] [MEDLINE] [ChemPort]
  8. R. Imbihl, M. P. Cox, and G. Ertl, J. Chem. Phys. 84, 3519 (1986). [ISI] [ChemPort]
  9. M. Eiswirth and G. Ertl, Surf. Sci. 177, 90 (1986). [Inspec] [ISI] [ChemPort]
  10. S. B. Schwartz and L. D. Schmidt, Surf. Sci. 183, L269 (1987). [ISI] [ChemPort]
  11. S. Ladas, R. Imbihl, and G. Ertl, Surf. Sci. 198, 42 (1988). [ISI] [ChemPort]
  12. P. R. Norton, P. E. Bindner, K. Griffiths, T. E. Jackman, J. A. Davies, and J. Rüstig, J. Chem. Phys. 80, 3859 (1984). [ISI] [ChemPort]
  13. R. C. Yeates, J. E. Turner, A. J. Gellman and G. A. Somorjai, Surf. Sci. 149, 175 (1985). [ISI] [ChemPort]
  14. M. Ehsasi, J. H. Block, K. Christmann, and W. Hirschwald, J. Vac. Sci. Technol. A 5, 821 (1987).
  15. R. Imbihl, M. P. Cox, G. Ertl, H. Müller, and W. Brenig, J. Chem. Phys. 83, 1578 (1985).
  16. P. Möller, K. Wetzl, M. Eiswirth, and G. Ertl, J. Chem. Phys. 85, 5328 (1986). [ISI]
  17. S. Ladas, R. Imbihl, and G. Ertl, Surf. Sci. 197, 153 (1988). [ISI] [ChemPort]
  18. M. Eiswirth, R. Schwankner, and G. Ertl, Z. Phys. Chem. N. F. 144, 59 (1985).
  19. See, for example, R. P. H. Gasser, An Introduction of Chemisorption and Catalysis by Metals (Clarendon, Oxford, 1985).
  20. M. Eiswirth, K. Krischer, and G. Ertl, Surf. Sci. 202, 565 (1988). [Inspec] [ISI] [ChemPort]
  21. S. Ladas, R. Imbihl, and G. Ertl (in preparation).
  22. R. J. Schwankner, M. Eiswirth, P. Möller, K. Wetzl, and G. Ertl, J. Chem. Phys. 87, 742 (1987). [ISI]
  23. M. Eiswirth, Thesis, University of Munich, 1987.
  24. M. Eiswirth and G. Ertl, Phys. Rev. Lett. 60, 1526 (1988). [MEDLINE] [ChemPort]
  25. M. Wilf and P. T. Dawson, Surf. Sci. 65, 399 (1977). [Inspec] [ISI] [ChemPort]
  26. R. Ducros and R. P. Merrill, Surf. Sci. 55, 227 (1976). [Inspec] [ISI] [ChemPort]
  27. V. S. Sundaram and P. H. Dawson, Surf. Sci. 146, L593 (1984). [Inspec]
  28. N. Freyer, M. Kiskinova, G. Pirug, and H. P. Bonzel, Surf. Sci. 166, 206 (1986). [Inspec] [ISI] [ChemPort]
  29. See Refs. 15 and 16 for a compilation of the relevant literature.
  30. P. Möller, Thesis, University of Munich, 1987.
  31. K. Heinz, A. Barthel, L. Hammer, and K. Müller, Surf. Sci. 191, 174 (1987). [Inspec]
  32. (a) R. Dagonnier, M. Dumont, and J. Nuyts, J. Catal. 66, 130 (1980);
    33. (b) J. P. Dath and J. P. Dauchot, J. Catal. 97, 100 (1986);
    (c) M. Ehsasi, Thesis, FU Berlin, 1988 (in preparation).
  33. R. J. Behm, P. A. Thiel, P. R. Norton, and G. Ertl, J. Chem. Phys. 78, 7437, 7448 (1983). [ChemPort]
  34. (a) J. Fair and R. I. Madix, J. Chem. Phys. 73, 3480 (1980); [ISI] [ChemPort]
    35. (b) P. Hofmann, S. R. Bare, and D. A. King, Surf. Sci. 117, 245 (1982); [Inspec] [ISI]
    (c) T. E. Jackman, J. A. Davies, D. P. Jackson, W. N. Unertl, and P. R. Norton, Surf. Sci. 120, 389 (1982). [Inspec]
  35. (a) G. Padberg and E. Wicke, Chem. Eng. Sci. 22, 1035 (1967); [ChemPort]
    36. (b) N. I. Jaeger, K. Möller, and P. J. Plath, J. Chem. Soc. Faraday Trans 1 82, 3315 (1986); [ISI] [ChemPort]
    (c) J. R. Brown, G. A. D'Netto, and R. A. Schmitz, in Temporal Order, edited by L. Rensing and N. I. Jaeger (Springer, Heidelberg, 1985) p. 86;
    (d) D. J. Kaul and E. E. Wolf, J. Catal. 91, 216 (1985); [ISI] [ChemPort]
    93, 321 (1985); [ChemPort]
    (e) R. Sant and E. E. Wolf (to be published);
    (f) H. U. Onken, Thesis, University of Münster, 1987;
    H. U. Onken and E. Wicke (to be published);
    (g) J. P. Dath and J. P. Dauchot, J. Catal. (tobe published).
  36. See, for example, Oscillations and Travelling Waves in Chemical Systems, edited by R. J. Field and M. Berger (Wiley, New York, 1985).
  37. P. K. Tsai, M. B. Maple, and R. K. Herz, J. Catal. (to be published).

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