Electrode Potential Dependence of Elementary Reaction Steps in Electrocatalysis: Development of Ab Initio Methodology and Applications

电催化的基本步骤的计算研究形成了分析和表面化学计划支持的这个研究项目的重点。 阿尔弗雷德教授B。 安德森的研究小组在凯斯西方应用从头计算量子力学计算的电子和质子转移的电化学界面的研究。 用密度泛函相关校正方法研究了氧在铂电极表面的四电子还原成水和CO在铂电极表面被水和羟基氧化的反应。 电极电位的依赖性的基本反应步骤是强调，并与合作者进行的实验研究在凯斯Western.To了解电极反应的详细微观机制重要的电催化和燃料电池的设计，量子化学计算进行了比较，以确定电极表面上的分子过程的动力学和能量途径。 本计画由分析与表面化学计画所赞助，针对微观反应机制的问题。 凯斯西方的安德森教授的小组研究了氧气的还原和CO的氧化，作为这些电催化过程的重要模型系统。 这些研究的信息将有助于燃料电池和电催化系统的设计和工程。

Calculational studies of the elementary steps of electrocatalysis form the focus of this research project supported in the Analytical and Surface Chemistry Program. Professor Alfred B. Anderson's research group at Case Western applies ab initio quantum mechanical calculations to the study of electron and proton transfer at the electrochemical interface. Density functional correlation corrected methods are used to examine the four electron reduction of oxygen to water and the oxidation of CO by water and hydroxyl at the platinum electrode surface. The electrode potential dependence of the fundamental reaction steps is emphasized, and comparisons with experimental studies carried out by collaborators at Case Western are included.In order to understand the detailed microscopic mechanism of electrode reactions important to electrocatalysis and fuel cell design, quantum chemical calculations are used to determine the kinetic and energetic pathways for molecular processes on the electrode surface. This project, supported by the Analytical and Surface Chemistry Program, addresses these questions of microscopic reaction mechanism. Professor Anderson's group at Case Western examines the reduction of oxygen and the oxidation of CO as important model systems for these electrocatalytic processes. Information from these studies will be useful in the design and engineering of fuel cell and electrocatalytic systems.