Mean Field Approximation of Langmuir-Hinshelwood CO-Surface Reactions Considering Lateral Interactions

被引:7
作者
Gomez-Marin, Ana Ma. [1 ]
Hernandez-Ortiz, Juan P. [2 ,3 ]
机构
[1] Univ Nacl Colombia, Dept Quim & Petroleos, Medellin, Colombia
[2] Univ Nacl Colombia, Dept Mat, Medellin, Colombia
[3] Univ Wisconsin, Dept Chem & Biol Engn, Madison, WI 53706 USA
关键词
SINGLE-CRYSTAL ELECTRODES; MONTE-CARLO SIMULATIONS; LATTICE-GAS MODEL; CARBON-MONOXIDE; ELECTROCHEMICAL OXIDATION; INFRARED-SPECTROSCOPY; COMPETITIVE ADSORPTION; MONOLAYER OXIDATION; ADLAYER STRUCTURES; KINETIC THEORY;
D O I
10.1021/jp404711p
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 mean field approximation to model the CO electrocatalytic oxidation on metal surfaces, including attractive and repulsive effective lateral interactions between the species, is employed. Adsorbed CO reacts with adsorbed OH from water dissociation through a Langmuir-Hinshelwood mechanism. Simulated results suggest alternative explanations to experimental observations during CO stripping oxidation on different electrodes by potential step chronoamperometry or voltammetry. Even though the model ignores higher order interactions, such as three-body or long-ranged interactions, the results extend the conceptual framework for transient kinetics and stripping voltammograms for CO oxidation on metallic surfaces or any other electrochemical Langmuir-Hinshelwood reaction. In spite of the high level of simplicity, the model is a promising tool for the understanding of the electrocatalytic activity and results were qualitatively compared with experimental results.
引用
收藏
页码:15716 / 15727
页数:12
相关论文
共 71 条
[51]   Some interpretations of surface vibrational spectroscopy pertinent to fuel-cell electrocatalysis [J].
Park, S ;
Wasileski, SA ;
Weaver, MJ .
ELECTROCHIMICA ACTA, 2002, 47 (22-23) :3611-3620
[52]   Kinetics of electrooxidation of a CO monolayer at the platinum/electrolyte interface [J].
Petukhov, AV ;
Akemann, W ;
Friedrich, KA ;
Stimming, U .
SURFACE SCIENCE, 1998, 402 (1-3) :182-186
[53]   Effect of molecular mobility on kinetics of an electrochemical Langmuir-Hinshelwood reaction [J].
Petukhov, AV .
CHEMICAL PHYSICS LETTERS, 1997, 277 (5-6) :539-544
[54]   The electrochemical oxidation of carbon monoxide adsorbed on Pt(111) in aqueous electrolytes as monitored by in situ potential step-second harmonic generation [J].
Pozniak, B ;
Mo, Y ;
Scherson, DA .
FARADAY DISCUSSIONS, 2002, 121 :313-322
[55]   Rate laws for reductive stripping of NO adlayers at single-crystal platinum electrodes as deduced from transient experiments [J].
Rosca, V ;
Koper, MTM .
SURFACE SCIENCE, 2005, 584 (2-3) :258-268
[56]   CO ADSORBATE ON PT(111) SINGLE-CRYSTAL SURFACES [J].
SANTOS, E ;
LEIVA, EPM ;
VIELSTICH, W .
ELECTROCHIMICA ACTA, 1991, 36 (3-4) :555-561
[57]   Modeling base voltammetry and CO electrooxidation at the Pt(111)-electrolyte interface: Monte Carlo simulations including anion adsorption [J].
Saravanan, C ;
Koper, MTM ;
Markovic, NM ;
Head-Gordon, M ;
Ross, PN .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2002, 4 (12) :2660-2666
[58]   Stripping and bulk CO electro-oxidation at the Pt-electrode interface: Dynamic Monte Carlo simulations [J].
Saravanan, C ;
Markovic, NM ;
Head-Gordon, M ;
Ross, PN .
JOURNAL OF CHEMICAL PHYSICS, 2001, 114 (14) :6404-6412
[59]   ESTIMATING SURFACE-DIFFUSION COEFFICIENTS [J].
SEEBAUER, EG ;
ALLEN, CE .
PROGRESS IN SURFACE SCIENCE, 1995, 49 (03) :265-330
[60]   Mechanism of CO oxidation on Pt(111) in alkaline media [J].
Spendelow, J. S. ;
Goodpaster, J. D. ;
Kenis, P. J. A. ;
Wieckowski, A. .
JOURNAL OF PHYSICAL CHEMISTRY B, 2006, 110 (19) :9545-9555