Alkane Oxidation Chemistry on Rh(111): The Relationship between Oxygen Coverage and Partial Oxidation

部分氧化催化是一个经济上重要但科学上知之甚少的过程。阐明部分氧化催化的机理，特别是甲烷和其他烷烃的活化，是本研究项目的重点，由分析和表面化学计划支持。在氧覆盖的Rh（111）单晶表面上进行的模型反应用于探索部分氧化反应的机理。高分辨率电子能量损失光谱结合热解吸光谱提供了烷烃在Rh（111）表面氧化的机理和动力学信息，作为氧覆盖的函数。研究中采用了一系列制备和检测这些反应中可能的自由基中间体的方法。更好地了解这一过程可能会对设计利用大量甲烷能源储备的催化剂产生影响。了解部分氧化催化，特别是甲烷的活化及其转化为甲醇或合成气，可能会产生巨大的经济影响，因为可利用的甲烷储量很大。本研究项目通过研究适当模型催化系统的动力学和机制来发展这种理解。

Partial oxidation catalysis is an economically important but scientifically poorly understood process. The elucidation of the mechanism of partial oxidation catalysis, particularly the activation of methane and other alkanes, forms the focus of this research project supported by the Analytical and Surface Chemistry Program. Model reactions carried out on oxygen covered Rh(111) single crystal surfaces are used to probe the mechanism of the partial oxidation reaction. High resolution electron energy loss spectroscopy combined with thermal desorption spectroscopy provide information about the mechanism and kinetics of alkane oxidation on the Rh(111) surface as a function of oxygen coverage. A range of methods for preparing and examining possible radical intermediates in these reactions are employed in the studies. A better understanding of this process could have impact on the design of catalysts for utilization of vast methane energy reserves. An understanding of partial oxidation catalysis, particularly the activation of methane and its conversion to methanol or synthesis gas, could have enormous economic impact due to the large reserves of methane available. This research project works to develop this understanding, by examining the kinetics and mechanisms of appropriate model catalytic systems.