A REACTIVE PHASE-DIAGRAM OF CO OXIDATION ON PD(110) - STEADY AND OSCILLATORY STATES

被引:46
作者
EHSASI, M
BERDAU, M
REBITZKI, T
CHARLE, KP
CHRISTMANN, K
BLOCK, JH
机构
[1] Fritz-Haber-Institut der MPG, D-14195 Berlin-Dahlem
[2] Freie Universität Berlin, Institut für Physikalische und Theoretische Chemie, D-1000 Berlin 33
关键词
D O I
10.1063/1.464425
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 steady and oscillatory regions of the CO oxidation reaction on the Pd (110) surface have been determined as a function of externally controlled parameters (flow rate, CO and oxygen partial pressures, temperature) over a wide range. At constant sample temperature and flow rate, the experiments yield a characteristic cross-shaped phase diagram separating regions of monostability, bistability, and oscillatory behavior. The existence of a cross-shaped phase diagram indicates the operation of a slow feedback process, which could be traced back to the (experimentally verified) formation and retarded removal of subsurface oxygen during the reaction. The diagram reflects one of the first well-defined oscillatory systems in heterogeneous catalysis and may provide a general basis for mechanistic studies and models of oscillatory surface reactions.
引用
收藏
页码:9177 / 9184
页数:8
相关论文
共 45 条
[1]   MATHEMATICAL-MODELING OF KINETIC OSCILLATIONS IN THE CATALYTIC CO OXIDATION ON PD(110) - THE SUBSURFACE OXYGEN MODEL [J].
BASSETT, MR ;
IMBIHL, R .
JOURNAL OF CHEMICAL PHYSICS, 1990, 93 (01) :811-821
[2]  
BELOUSOV BP, 1958, SB REF RAD MEDITSIN
[3]   THERMALLY AND KINETICALLY PRODUCED INSTABILITIES IN REACTION BEHAVIOR OF INDIVIDUAL CATALYST GRAINS [J].
BEUSCH, H ;
WICKE, E ;
FIEGUTH, P .
CHEMIE INGENIEUR TECHNIK, 1972, 44 (07) :445-&
[4]  
BEUSCH H, 1972, ADV CHEM, V109, P615
[5]   SIMPLEST CATALYTIC MECHANISM PERMITTING SEVERAL STEADY STATES OF SURFACE [J].
BYKOV, VI ;
ELOKHIN, VI ;
YABLONSKII, GS .
REACTION KINETICS AND CATALYSIS LETTERS, 1976, 4 (02) :191-198
[6]   A SYSTEMATICALLY DESIGNED HOMOGENEOUS OSCILLATING REACTION - THE ARSENITE-IODATE-CHLORITE SYSTEM [J].
DEKEPPER, P ;
EPSTEIN, IR ;
KUSTIN, K .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1981, 103 (08) :2133-2134
[7]   THEORETICAL AND EXPERIMENTAL-ANALYSIS OF PHASE-DIAGRAMS AND RELATED DYNAMICAL PROPERTIES IN THE BELOUSOV-ZHABOTINSKII SYSTEM [J].
DEKEPPER, P ;
BOISSONADE, J .
JOURNAL OF CHEMICAL PHYSICS, 1981, 75 (01) :189-195
[8]  
EHSASI M, 1989, SURF SCI, V210, pL198, DOI 10.1016/0039-6028(89)90593-1
[9]   REACTION-RATE OSCILLATION OF CO OXIDATION ON PT(210) [J].
EHSASI, M ;
REZAIESEREJ, S ;
BLOCK, JH ;
CHRISTMANN, K .
JOURNAL OF CHEMICAL PHYSICS, 1990, 92 (12) :7596-7609
[10]  
Ehsasi M., 1989, Journal of Chemical Physics, V91, P4949, DOI 10.1063/1.456736