Experimental Studies of Gas Phase Reactions of Transition Metals with Simple Hydrocarbons: Vibrationally Resolved Anion Photoelectron Spectroscopy of Flow Tube Reaction Products

在这个由化学系化学结构，动力学和机制计划资助的项目中，Doreen Leopold教授和她的团队将研究小过渡金属簇合物的结构和反应性。 气相金属物种将在流管反应器中制备，并且它们与不饱和有机分子反应的质量选择性阴离子产物将通过阴离子光电子能谱法探测。 对于裸金属簇和金属配体配合物，这些结果将提供电子亲合势，电子态能量和振动频率的测量。 除了对直接参与这些实验的研究人员进行培训外，更广泛的影响活动还将包括继续领导一项新的教学导师计划，该计划面向对学术生涯感兴趣的研究生和博士后，以及改进计算器的方法的发展-普通化学本科生的自由数学流利。这些实验将产生有机金属自由基的光谱信息，可以作为模型对于过渡金属催化剂反应中的中间体，将有助于阐明结构-反应性关系。 此外，这些对小的、定义明确的簇的研究将提供实验基准，以帮助其他研究人员开发改进的计算方法来处理更直接技术相关的较大金属纳米系统。

In this project, funded by the Chemical Structure, Dynamics and Mechanisms Program of the Chemistry Division, Professor Doreen Leopold and her group will investigate the structures and reactivities of small transition metal clusters. Gas phase metal species will be prepared in a flow tube reactor, and mass-selected anionic products of their reactions with unsaturated organic molecules will be probed by anion photoelectron spectroscopy. For the bare metal clusters and metal-ligand complexes, these results will provide measurements of electron affinities, electronic state energies, and vibrational frequencies. In addition to the training of researchers directly involved in these experiments, broader impact activities will include the continued leadership of a new teaching mentorship program for graduate students and postdoctorals interested in academic careers, and the development of methods to improve the calculator-free math fluencies of undergraduate general chemistry students.These experiments will yield spectroscopic information for organometallic radicals that may serve as models for intermediates in the reactions of transition metal catalysts, and will help to elucidate structure-reactivity relationships. In addition, these studies of small, well-defined clusters will provide experimental benchmarks to aid other researchers in developing improved computational methods to treat larger metal nanosystems of more direct technological relevance.