Structure Sensitivity of the Mechanism of Simple Catalytic Reactions of Hydrocarbons

摘要9403840理查德·梅赛尔这是一项关于金属表面催化反应结构敏感性的实验和理论相结合的研究。用超高真空表面光谱技术研究了简单烃类配体与一系列暴露在不同折射率面上的铂单晶之间的相互作用。将实验观测结果与密度泛函计算的结果进行了比较，并通过设计新的实验来迭代该过程以验证理论计算的预测。目标是确定控制碳氢化合物反应的关键相互作用，并描述这些相互作用如何从一个晶面到另一个晶面变化。人们早就知道，金属上各种反应的催化活性因晶面不同而不同；在许多情况下，暴露平面的分布是选择性的预测指标。虽然一些极端情况可以用原始的立体或几何论证来解释，但没有令人满意的理论框架来解决这个问题，这对化学、制药和燃料行业的许多过程都是至关重要的。这一努力满足了这一需求。***

ABSTRACT 9403840 Richard Masel This is a combined experimental and theoretical study of the structure sensitivity of catalytic reactions on metal surfaces. Ultrahigh-vacuum surface spectroscopic techniques are used to examine the interactions of simple hydrocarbon ligands with a series of platinum single crystals that expose various index planes. The experimental observations are compared to the results of density functional calculations, and the process iterated by designing new experiments to test predictions of the theoretical calculations. The objective is to identify the key interactions that control the reactions of hydrocarbons and describe how those interactions vary from one crystal face to another. It has long been known that catalytic activities for various reactions on metals vary from one crystal face to another; in many cases, the distribution of exposed planes is a predicter of selectivity. While some extreme cases can be explained by crude steric or geometric arguments, there is no satisfactory theoretical framework to address this issue, which is critical for many processes in the chemical, pharmaceutical, and fuel industries. This effort addresses that need. ***