Theoretical study of pattern formation during the catalytic oxidation of CO on Pt{100} at low pressures.

A. T. ANGHEL; R. B. HOYLE; I. M. IRURZUN; M. R. E. PROCTOR; D. A. KING

JOURNAL OF CHEMICAL PHYSICS

Año: 2007 vol. 127 p. 1647111 - 16471114

0021-9606

Theoretical studies have thus far been unable to model pattern formation during the reaction in this system on physically feasible length and time scales. In this paper, we derive a computational reaction-diffusion model for this system in which most of the input parameters have been determined experimentally. We model the surface on a mesoscopic scale intermediate between the microscopic size of CO islands and the macroscopic length scale of pattern formation. In agreement with experimental investigations [M. Eiswirth et al., Z. Phys. Chem., Neue Folge 144, 59 (1985)], the results from our model divide the CO and O2 partial pressure parameter space into three regions defined by the level of CO coverage or the presence of sustained oscillations. We see CO fronts moving into oxygen-covered regions, with the 1×1 to hex phase change occurring at the leading edge. There are also traveling waves consisting of successive oxygen and CO fronts that move into areas of relatively high CO coverage, and in this case, the phase change is more gradual and of lower amplitude. The propagation speed of these reaction waves is similar to those observed experimentally for CO and oxygen fronts [H. H. Rotermund et al., J. Chem. Phys. 91, 4942 (1989); H. H. Rotermund et al., Nature (London) 343, 355 (1990); J. Lauterbach and H. H. Rotermund, Surf. Sci. 311, 231 (1994)]. In the two-dimensional version of our model, the traveling waves take the form of target patterns emitted from surface inhomogeneities.