The Catalytic Oxidation Chemistry of Silver Surfaces

本研究的目的是鉴定烯烃在银（110）表面部分氧化和完全氧化的中间体，并定量这些过程中基本步骤的能量学。这包括，对于部分氧化，金属环中间体的生产，鉴定和表征，这些中间体与原子和分子吸附氧的催化氧化有关，对于完全氧化，丙烯燃烧机制的研究。电子能量损失光谱用于识别吸附的中间体并测量它们参与的反应速率。程序升温解吸被用于识别解吸产物和测量解吸速率。本研究中涉及的烯烃部分氧化工艺具有重要的商业意义，但目前只能应用于极少数烯烃。本研究结果可指导现有工艺的更好控制和产量的提高。更重要的是，它可能为将这种方法扩展到额外的烯烃指明道路，这将是一项技术突破。

The objectives of this study are the identification of intermediates in the partial and total oxidations of olefins on silver (110) surfaces, and quantification of the energetics of elementary steps in these processes. This includes, for partial oxidation, the production, identification, and characterization of the metallocycle intermediates relevant to catalytic oxidtion by both atomically and molecularaly adsorbed oxygen, and, for total oxidation , the investigation of the mechanism of propylene combustion. Electron energy loss spectroscopy is used to identify adsorbed intermediates and to measure the rates of reactions in which they participate, and temperature-programmed desorption is used to identify desorption products and to measure the rates of desorption. Partial oxidation of olefins, the process involved in this study, is of great commerical importance, but as presently practiced, can be applied only to a very few olefins. The results of this study could lead to better control and improved yields in the existing process. More significantly, it may point the way for extending this approach to additional olefins, which would represent a technological breakthough.