Dynamics of Organic Ion-Molecule Reactions in the Gas Phase

在这个由化学系教师早期职业发展(CALEAR)计划资助的项目中，卡内基梅隆大学化学系的Susan Graul教授将研究气相离子-分子反应的热化学、动力学和动力学。反应截面、产物角和能量分布将使用质量分析离子动能谱和引导离子束技术来确定。初步研究将集中在甲基卤化物CH3X(X=Cl，Br，I)与F-和Cl-离子的放热双分子亲核取代(SN2)反应。这些研究将扩展到其他体系，如F-和Cl-离子与氯乙腈和溴乙腈的反应等。此外，还将研究双分子消除反应。这些实验研究将得到相关反应中间体和过渡态的电子结构计算以及所研究反应的统计理论模型的补充，以便与实验结果进行比较。伴随着研究活动的是一种特定的教育努力，以适应全面、平衡、学术生涯的发展。离子-分子反应化学处于气相反应化学的前沿。因此，它在燃烧过程化学、高层大气化学和其他领域发挥着重要作用。这项研究将有助于我们理解这些过程，为发展先进的理论，基于分子的化学反应模型提供合适的数据。

In this project funded through the Faculty Early Career Development (CAREER) Program of the Chemistry Division, Professor Susan Graul of the Department of Chemistry of the Carnegie- Mellon University will study the thermochemistry, kinetics, and dynamics of gas-phase ion-molecule reactions. Reaction cross sections and product angular and energy distributions will be determined using mass-analyzed ion kinetic energy spectrometry and guided ion-beam techniques. Initial studies will focus on the exothermic bimolecular nucleophilic substitution (SN2) reactions of methyl halides CH3X (X=Cl,Br,I) with F- and Cl- ions. These studies will be extended to other systems such as the reactions of F- and Cl- ions with chloroacetonitrile and bromoacetonitrile, and others. Furthermore, bimolecular elimination reactions will also be investigated. These experimental studies will be complemented by electronic structure calculations for relevant reaction intermediates and transition states, and statistical theoretical modeling of the reactions studied for comparison with experimental results. Accompanying the research activity is a specified education effort appropriate to the development of a full, balanced, academic career. The chemistry of ion-molecule reactions is at the forefront of gas phase reaction chemistry. As such it plays an important role in the chemistry of combustion processes, the chemistry of the upper atmosphere, and other areas. This research will contribute to our understanding of these processes by providing data suitable for the development of advanced theoretical, molecular based models of chemical reactions.