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

部分氧化催化是一种经济上重要但科学上知之甚少的方法。 部分氧化催化机制的阐明，特别是甲烷和其他烷烃的活化，形成了分析和表面化学计划支持的本研究项目的重点。 用Rh（111）单晶表面氧覆盖的模型反应探讨了部分氧化反应的机理。 高分辨率电子能量损失谱结合热脱附谱提供了关于烷烃在Rh（111）表面上氧化的机制和动力学的信息，作为氧覆盖度的函数。 一系列的方法，用于制备和检查可能的自由基中间体在这些反应中采用的研究。更好地理解这一过程可能会对利用大量甲烷能源储备的催化剂的设计产生影响。 对部分氧化催化的理解，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，因为甲烷的储量很大。 该研究项目致力于通过研究适当的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.