Kinetic phase diagram for CO oxidation on Pt(210): Pattern formation in the hysteresis and oscillation regions

被引:18
作者
Berdau, M
Karpowicz, A
Yelenin, GG
Christmann, K
Block, JH
机构
[1] MOSCOW MV LOMONOSOV STATE UNIV,DEPT COMPUTAT MATH & CYBERNET,LAB MATH MODELING PHYS,MOSCOW 119899,RUSSIA
[2] FREE UNIV BERLIN,INST PHYS & THEORET CHEM,D-14195 BERLIN,GERMANY
关键词
D O I
10.1063/1.473131
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The reactive behavior of catalytic CO oxidation on Pt(210) is studied by means of combined reaction rate measurements and photoelectron emission microscopy (PEEM). These methods allow an investigation of the phenomena at macroscopic and mesoscopic level, respectively. The external control parameters (how rate, CO and oxygen partial pressures, surface temperature and scanning rates of pressure and temperature) are systematically varied to reveal various reactive regions in parameter space. The macroscopic measurements for a given temperature and flow rate (under isothermal conditions) show that lower pressures lead to a pronounced clockwise hysteresis in the production rate of CO2, while increasing pressures' cause a systematic narrowing leading to a crossing: of the two hysteresis branches into a region of counterclockwise hysteresis. A further pressure increase leads to macroscopic temporal oscillations. Mesoscopic spatiotemporal oscillations appear at the same conditions. The resulting macroscopic isothermal kinetic phase diagram exhibits a cross-shaped characteristic similar to that previously obtained 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 spatiotemporal patterns, such as islands, waves, target patterns and spirals, are correlated via the external control parameters with different regions in the macroscopic isothermal phase diagram. The results are compared with previous data of CO oxidation on other surfaces, like Pd(110) and Pt(110). (C) 1997 American Institute of Physics.
引用
收藏
页码:4291 / 4308
页数:18
相关论文
共 45 条
[21]   OSCILLATORY KINETICS IN HETEROGENEOUS CATALYSIS [J].
IMBIHL, R ;
ERTL, G .
CHEMICAL REVIEWS, 1995, 95 (03) :697-733
[22]   SPATIOTEMPORAL CONCENTRATION PATTERNS IN A SURFACE-REACTION - PROPAGATING AND STANDING WAVES, ROTATING SPIRALS, AND TURBULENCE [J].
JAKUBITH, S ;
ROTERMUND, HH ;
ENGEL, W ;
VONOERTZEN, A ;
ERTL, G .
PHYSICAL REVIEW LETTERS, 1990, 65 (24) :3013-3016
[23]   BIFURCATION-ANALYSIS OF AN OSCILLATING SURFACE-REACTION MODEL [J].
KRISCHER, K ;
EISWIRTH, M ;
ERTL, G .
SURFACE SCIENCE, 1991, 251 :900-904
[24]   SPATIOTEMPORAL PATTERN-FORMATION DURING THE CATALYTIC COOXIDATION ON PT(100) [J].
LAUTERBACH, J ;
ROTERMUND, HH .
SURFACE SCIENCE, 1994, 311 (1-2) :231-246
[25]  
LAUTERBACH J, COMMUNICATION
[26]  
MIKHAILOV AS, 1990, FDN SYNERGETICS, V1, pCH2
[27]  
MOLDENHAUER S, UNPUB
[28]   REACTION-DIFFUSION PATTERNS IN THE CATALYTIC COOXIDATION ON PT(110) - FRONT PROPAGATION AND SPIRAL WAVES [J].
NETTESHEIM, S ;
VONOERTZEN, A ;
ROTERMUND, HH ;
ERTL, G .
JOURNAL OF CHEMICAL PHYSICS, 1993, 98 (12) :9977-9985
[29]  
Nicolis G., 1977, SELF ORG NONEQUILIBR
[30]  
OUYANG Q, 1987, J PHYS CHEM-US, V91, P6040