Adsorbate Photochemical Dynamics and Catalysis

本研究项目探讨了在具有良好特征的固体表面上光诱导反应的详细动力学。弗吉尼亚大学的伊恩·哈里森教授和他的学生们利用角度分辨飞行时间的测量方法，正在探索N2、CO2和甲烷等吸附剂的光活化。在分析和表面化学计划的支持下，这项工作提供了对表面小分子活化机制的详细见解，对多相催化方法的发展和改进具有重要意义。这些吸附分子的电荷转移激发，然后对解吸产物进行分析，使该小组能够探测光刺激和热刺激表面反应的过渡状态的细节。吸附分子的光激发可以用来探测表面上更常见的热激活过程的动力学。该研究项目使用快速激光激发吸附物，然后进行角度分辨的产物速度测量，以提供有关几个重要的小分子反应的详细动力学信息，这些反应发生在特征良好的表面上。这些光动力学研究的结果随后被应用于理解相当重要的热活化催化反应的机制。

This research project addresses the detailed dynamics of photoinduced reactions at well-characterized solid surfaces. Using angle resolved time-of-flight measurements, Professor Ian Harrison and his students at the University of Virginia are exploring the photoactivation of adsorbates such as N2, CO2, and methane. With the support of the Analytical and Surface Chemistry Program this work provides detailed insight into the mechanisms of small molecule activation at surfaces, with strong implications for the development and improvement of heterogeneous catalytic methods. Charge transfer excitation of these adsorbed molecules followed by analysis of the desorbed products, allows this group to probe the details of the transition state for photostimulated as well as thermally stimulated surface reactions. The photoexcitation of adsorbed molecules can be used to probe the dynamics of more common thermally activated processes on surfaces. This research project uses fast laser excitation of adsorbates, followed by angle resolved measurements of product velocities to provide information about the detailed dynamics of several important small molecule reactions on well-characterized surfaces. The results of these photodynamic studies are then applied to the understanding of the mechanisms of thermally activated catalytic reactions of considerable importance.