S. Nettesheim et al., REACTION-DIFFUSION PATTERNS IN THE CATALYTIC COOXIDATION ON PT(110) -FRONT PROPAGATION AND SPIRAL WAVES, The Journal of chemical physics, 98(12), 1993, pp. 9977-9985
The dymanic behavior of elliptical front propagation and spiral-shaped
excitation concentration waves associated with the catalytic oxidatio
n of CO on a Pt(110)-surface was investigated by means of photoemissio
n electron microscopy (PEEM). The properties of these patterns can be
tuned through the control parameters, viz., the partial pressures of C
O and O2 and the sample temperature. Over a wide range of control para
meters the transition between two metastable states (COad and O(ad) co
vered surface) proceeds via nucleation and growth of elliptical reacti
on-diffusion (RD)-fronts. Front velocities and critical radii for nucl
eation are determined by the diffusion of adsorbed CO under reaction c
onditions. If at constant p(O2), T the CO partial pressure is increase
d beyond a critical value a transition to qualitatively different dyna
mic behavior takes place. The elliptical fronts give way to oxygen spi
ral waves of excitation spreading across the CO-covered areas. For fix
ed experimental conditions a broad distribution of spatial wavelengths
and temporal rotation periods was found. This effect has to be attrib
uted to the existence of surface defects of mum-size to which the spir
al tip is pinned. These data lead to a dispersion relation between the
front propagation velocity and the wavelength, respectively, period.
In addition, the dynamics of free spiral-shaped excitation waves was i
nvestigated under the influence of externally modulated temperature. N
ow the spiral starts to drift, resulting in distortion of the Archimed
ian shape and a pronounced Doppler effect.