Structure Sensitivity of the Hydrogenolysis of Simple Hydro-carbons on Platinum Single Crystals

这是正在进行的研究的延续，目的是测试配位化学的某些原理在多大程度上可以应用于表面反应；已经证明，轨道对称守恒原理可以将氧化氮或乙烯在铂上分解的速率变化作为折射率面（晶面）的函数进行建模。在本研究中，这被扩展到铂上碳氢化合物的氢解；研究了乙烷、乙烯、环丙烷、环丁烷和环戊烷。过去的研究表明，通过这一系列结构敏感性的变化令人费解。试图解释这些将使用理论和实验方法相结合，包括电子能量损失光谱，温度程序解吸，扫描隧道显微镜，放射性示踪剂研究和化学动力学。预测灵敏度和能量学的能力对于在分子水平上设计和控制催化过程是必不可少的。同时也涉及到环境控制、材料稳定性和性能等方面的问题。

This is a continuation of ongoing research to test the extent to which certain principles from coordination chemistry can be applied to surface reactions; it has already been shown that the principle of conservation of orbital symmetry can model the variation in rates as a function of index plane (crystal face) for the decomposition of either nitric oxide or ethylene on platinum. In this study, this is extended to hydrogenolysis of hydrocarbons on platinum; ethane, ethylene, cyclopropane, cyclobutane, and cyclopentane are studied. Past studies show puzzling variation in structure sensitivity through this series. An attempt to explain these will be made using a combination of theoretical and experimental approaches, including electron energy-loss spectroscopy, temperature-programmed desorption, scanning tunnelling microscopy, radiotracer studies, and chemical kinetics. The ability to predict sensitivity and energetics is essential for design and control of catalytic processes at the molecular level. It is also pertinent to other problems in environmental control and materials stability and performance.