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Mechanistic Principles of Platinum Oxide Formation and Reduction

机译：氧化铂形成与还原的机理原理

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摘要

In polymer electrolyte fuel cells, the platinum catalyst in its active form is found predominantly in an oxidized state. Formation and reduction of surface oxide species determine both the electrocatalytic activity of the oxygen reduction reaction as well as the rate of corrosive Pt dissolution. Understanding of mechanisms and rates of oxide formation and reduction is therefore essential in view of both performance and durability. Pt(111) is the generic model system for fundamental studies in fuel cell electrochemistry and cyclic voltammetry at Pt(111) gives an unabated view of the oxide formation and reduction processes. The unresolved challenge is to develop an electrochemical kinetic model that allows the current response measured in cyclic voltammetry to be de-convoluted and interpreted in relation to independent spectroscopic, imaging and theoretical data. Accordingly, a kinetic model for Pt(111) oxide formation and reduction within the voltage range of 0.65-1.15 V is developed and evaluated against electrochemical, spectroscopic and computational studies. Considering the complexity of surface processes involved and the simplicity of the proposed model, the agreement with the extensive range of data is convincing. The model provides a comprehensive picture of surface electrochemical processes that occur at Pt(111) in the normal operational voltage range of the cathode catalyst for polymer electrolyte fuel cells in automotive applications.
机译：在聚合物电解质燃料电池中，发现其活性形式的铂催化剂主要处于氧化态。表面氧化物种类的形成和还原既决定了氧还原反应的电催化活性，又决定了腐蚀性Pt的溶解速率。因此，从性能和耐用性两方面来理解氧化物形成和还原的机理和速率至关重要。 Pt（111）是在Pt（111）进行燃料电池电化学和循环伏安法基础研究的通用模型系统，提供了氧化物形成和还原过程的完整视图。尚未解决的挑战是开发一种电化学动力学模型，该模型可以对在循环伏安法中测得的电流响应进行反卷积并相对于独立光谱，成像和理论数据进行解释。因此，建立了动力学模型，用于在0.65-1.15 V的电压范围内形成和还原Pt（111）氧化物，并针对电化学，光谱和计算研究进行了评估。考虑到所涉及的表面过程的复杂性和所提出模型的简单性，令人信服的数据范围广泛。该模型为汽车应用中聚合物电解质燃料电池的阴极催化剂的正常工作电压范围内的Pt（111）处发生的表面电化学过程提供了全面的图像。

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