M. Berdau et al., KINETIC PHASE-DIAGRAM FOR CO OXIDATION ON PT(210) - PATTERN-FORMATIONIN THE HYSTERESIS AND OSCILLATION REGIONS, The Journal of chemical physics, 106(10), 1997, pp. 4291-4308
The reactive behavior of catalytic CO oxidation on Pt(210) is studied
by means of combined reaction rate measurements and photoelectron emis
sion microscopy (PEEM). These methods allow an investigation of the ph
enomena at macroscopic and mesoscopic level, respectively. The externa
l control parameters (how rate, CO and oxygen partial pressures, surfa
ce temperature and scanning rates of pressure and temperature) are sys
tematically varied to reveal various reactive regions in parameter spa
ce. The macroscopic measurements for a given temperature and flow rate
(under isothermal conditions) show that lower pressures lead to a pro
nounced clockwise hysteresis in the production rate of CO2, while incr
easing pressures' cause a systematic narrowing leading to a crossing:
of the two hysteresis branches into a region of counterclockwise hyste
resis. A further pressure increase leads to macroscopic temporal oscil
lations. Mesoscopic spatiotemporal oscillations appear at the same con
ditions. The resulting macroscopic isothermal kinetic phase diagram ex
hibits a cross-shaped characteristic similar to that previously obtain
ed for the Pd(110) surface. The mesoscopic lateral distribution of CO
and oxygen adsorbed on the surface is monitored with the photoelectron
emission microscope during the reaction at isothermal conditions and
different constant oxygen pressures. The observed mesoscopic spatiotem
poral patterns, such as islands, waves, target patterns and spirals, a
re correlated via the external control parameters with different regio
ns in the macroscopic isothermal phase diagram. The results are compar
ed with previous data of CO oxidation on other surfaces, like Pd(110)
and Pt(110). (C) 1997 American Institute of Physics.