Kinetics and Energetics of Gas Phase Metal Cluster Catalysis

在这个由化学部实验物理化学项目支持的项目中，Ervin将研究气相过渡金属团簇和吸附剂之间的相互作用。利用能量分辨碰撞诱导离解和时间分辨光解实验测量了吸附物在团簇上的结合能。将统计速率理论应用于簇解离数据，得到解吸能。主要推力包括光解动力学技术的开发，以获得裸金属团簇和团簇上吸附物的结合能；气相过渡金属团簇作为实际催化剂的探索以及与催化相关的小簇/配体系统的研究。一个引导离子束串联质谱计将用于收集数据。本项目测量的数据对于确定催化反应机理和绘制反应路径具有重要意义。这里研究的团簇是催化系统的模型，因为它们模拟了工业过程中催化剂中组成反应中心的小金属晶体。气相簇本身也可以作为催化剂，如铂簇阴离子将一氧化碳氧化为二氧化碳。

In this project supported by the Experimental Physical Chemistry Program of the Chemistry Division, Ervin will investigate the interactions between gas-phase transition metal clusters and adsorbates. Energy-resolved collision-induced dissociation and time-resolved photodissociation experiments are used to measure the binding energies of adsorbates on the clusters. Statistical rate theory is applied to the cluster dissociation data to obtain desorption energies. Major thrusts include exploitation of photodissociation dynamics techniques to obtain binding energies of bare metal clusters and of adsorbates on clusters; exploration of gas-phase transition metal clusters as actual catalysts; and examination of small cluster/ligand systems of relevance to catalysis. A guide ion beam tandem mass spectrometer will be used to gather the data.The data measured in this project are important for determining catalytic reaction mechanisms and for mapping out reaction paths. The clusters under study here are models for catalytic systems because they mimic small metal crystallites that comprise the reaction centers in catalysts used in industrial processes. Gas phase clusters themselves can also act as catalysts, as in the oxidation of carbon monoxide to carbon dioxide by platinum cluster anions.