Electro-oxidation of CO on Pt-based electrodes simulated by electronic structure calculations

被引：18

作者：

Saravanan, C

Dunietz, BD ^{[1
]}

Markovic, NM

Somorjai, GA

Ross, PN

Head-Gordon, M

机构：

[1] Univ Calif Berkeley, Lawrence Berkeley Lab, Div Sci Mat, Berkeley, CA 94720 USA

[2] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA

来源：

JOURNAL OF ELECTROANALYTICAL CHEMISTRY | 2003年 / 554卷

基金：

美国国家科学基金会;

关键词：

CO electro-oxidation; ab initio calculations; Pt surface catalysis; density functional theory calculations;

D O I：

10.1016/S0022-0728(03)00414-5

中图分类号：

O65 [分析化学];

学科分类号：

070302 ; 081704 ;

摘要：

CO electro-oxidation on Pt-based electrodes is simulated by density functional calculations on cluster models. A surface bound complex of CO with OH is identified as a crucial intermediate in the mechanism of CO oxidation. The complex under the influence of an appropriate potential and in the presence of water undergoes CO oxidation. The potential energy surface for this reaction as a function of the potential of the electrode is presented, and the barrier for the reaction is shown to vanish above a sufficiently positive applied potential. In addition, the different major barriers for the process are highlighted by comparing the mechanism on pure Pt to a Ru-Pt alloy. (C) 2003 Elsevier B.V. All rights reserved.

引用

页码：459 / 465

页数：7

共 41 条

[1] Quantum chemical approach to redox reactions including potential dependence: Application to a model for hydrogen evolution from diamond [J].