Catalysis and Separations with One Hand

本项目的目标是探索手性金属表面对映体选择化学的基本方面。研究的重点是由铜和铂等金属的高密勒指数面形成的自然手性表面。这些表面的手性源于三个低Miller指数微面相交形成的扭折阶梯状结构。在这个意义上，这种类型的表面手性不同于传统的以手性配体为模板的表面方法所赋予的手性。过去的工作已经探索了天然手性表面的结构，对映体特定的吸附几何结构，以及对映体特定的表面反应能。手性表面的这些性质决定了催化反应和色谱分离的对映选择性。这项工作的重点是利用实验和理论相结合的方法来探索各种结构的自然手性表面。虽然手征高密勒指数曲面的数量是无限的，但它们是由有限类型的扭结阶梯结构组成的。这项拟议的研究将通过使用以前表现出对映异构体表面化学的手性吸附来探索这组结构在铜单晶表面上的对映体专一性。教育活动预计将是对研究生的传统辅导。这项工作的基本目标是对一组高度特征化的自然手性表面上的对映选择性的根源提供一个基本的理解。

The objective of this project is to explore the fundamental aspects of enantioselectivechemistry on chiral metal surfaces. The investigation is focused on naturally chiral surfaces formed from high Miller index planes of metals such as Cu and Pt. The chirality of these surfaces arises from the kink-step-terrace structures that are formed by the intersections of three low Miller index microfacets. In this sense this type of surface chirality is distinct from the chirality imparted by the traditional approach of templating a surface with chiral ligands. Past work has probed the structure of naturally chiral surfaces, enantiospecific adsorbate geometries, and enantiospecific surface reaction energetics. These properties of chiral surfaces determine the enantioselectivities of catalytic reactions and chromatographic separations. The work proposed focuses on the exploration of naturally chiral surfaces of various structures using a combination of experimental and theoretical methods. Although there are an infinite number of chiral high Miller index surfaces, they are composed of a finite number of types of kink-step-terrace structures. The proposed investigation will explore the enantiospecificity of this set of structures on Cu single crystal surfaces by using chiral adsorbates that have previously exhibited enantiospecific surface chemistry. The educational activities are expected to be the traditional mentoring of graduate students. The fundamental goal of the proposed work is to provide a basic understanding of the roots of enantioselectivity on a set of highly characterized, naturally chiral surfaces.