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Quantitative Coordination-Activity Relations for the Design of Enhanced Pt Catalysts for CO Electro-oxidation

机译：CO电氧化增强Pt催化剂设计的定量配位关系

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摘要

Efficient redox transformations of CO are vital for remediating the imbalance of the biogeochemical cycle of carbon and also for the development of next-generation energy technologies such as fuel cells. For instance, CO oxidation is ubiquitous in hydrocarbon-based fuel cells and determines to a large extent their efficiency. As Pt is used in these cells, minimal catalyst loadings that do not compromise the activity are needed. In view of that, we present here a "coordination-activity plot" and electrochemical experiments on electro-oxidation of adsorbed CO to CO2 to establish quantitative structure activity relations for various Pt electrodes. We predict theoretically and verify experimentally that catalytic CO oxidation is enhanced by creating surface defects with optimal coordination, without alloying. Both largely overcoordinated and undercoordinated defects on Pt (at rough surfaces with cavities and metal adatoms, respectively) hinder the reaction, so that the maximal activity is reached on sites with a generalized coordination of (CN) over bar = 5.4. Importantly, this moderate coordination is found at defects such as step edges of electrodes with relatively short terrace lengths of 3-4 metal atoms.
机译：有效的CO的氧化还原转化对于修复碳生物地球化学循环的不平衡以及用于开发诸如燃料电池的下一代能源技术的开发至关重要。例如，共氧化在基于烃基燃料电池中普遍存在，并且在很大程度上决定了它们的效率。随着PT用于这些细胞中，需要不损害活性的最小催化剂载量。鉴于此，我们在此存在“协调活性图”和电化学实验的吸附CO至CO2的电氧化，建立各种PT电极的定量结构活性关系。我们在理论上预测并通过实际预测并通过在没有合金化的情况下产生具有最佳配位的表面缺陷来提高催化共氧化。在很大程度上在Pt（分别具有空腔和金属染色剂的粗糙表面上的粗糙表面上的缺陷均妨碍反应，从而在具有（CN）上的甲= 5.4上的普遍配位达到最大活性。重要的是，这种中等协调被发现在诸如电极的缺陷等缺陷中，具有相对短的露台长度为3-4金属原子。

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