Free radical chemistry in green solvents and development of novel spectroscopic techniques to study transient intermediates

我们想在室温离子液体和亚、超临界流体中进行化学动力学的研究。离子液体几乎完全由离子组成，而超临界流体是任何高于其临界温度和压力的流体，其中没有明显的气相和液相。从长远来看，我们的研究将为我们提供有用的信息，以设计既经济又环保的新型工业流程。特别是，我们将能够在寻找超临界流体基过程的最佳热力学条件或离子液体基过程中的离子液体类型方面做出贡献。在我们的许多研究中，我们使用μ子，从化学的角度来看，μ子可以被认为是轻质子。我们还想扩展我们最近开发的一项新技术，激光泵μ子探针技术，用于研究原子氢反应在激发态的动力学同位素效应，探测电离辐射过程中的瞬态，以及激发态的自由基中间体。我们还希望开发其他新的光谱方法。其中一种方法是发展电化学- μ子光谱技术，以便电化学地生产新的反应中间体，或者使用电化学方法和μ子辐照的结合。然后，我们将通过μ子方法通过原子核与未配对电子的耦合（超精细相互作用）来研究这些反应中间体的电子结构。我将继续在我们使用的两个主要设施，加拿大温哥华的TRIUMF国家实验室和英国的卢瑟福阿普尔顿实验室，使用跨学科的设置和最先进的实验工具，结合计算化学方法和传统的实验室方法，为参与本研究项目的本科生和研究生提供一个独特的训练环境。对于超临界流体和离子液体的研究，我们将重点提供与自由基化学和分子间相互作用相关的机械和动力学信息，这些信息与潜在的化学和制造业有关。

We would like to conduct studies of chemical dynamics in room temperature ionic liquids and in sub- and supercritical fluids. Ionic liquids are almost completely made of ions, while a supercritical fluid is any fluid above its critical temperature and pressure where there is no distinct gas and liquid phase. Our studies, in the long term, will give us information that will be useful to design novel industrial processes that are both economical and environmentally-friendly. In particular, we will be able to contribute in finding the optimum thermodynamic conditions for supercritical fluid based processes or types of ionic liquids in ionic liquid based processes. For many of our studies we use muons which from a chemical point of view can be considered as light protons. We would also like to expand a new technique, laser-pump muon probe technique, that we have recently developed to study the Kinetic Isotope Effects of atomic hydrogen reactions in the exited states, to probe transients in ionizing radiation processes, as well as free radical intermediates in excited states. We would also like to develop other novel spectroscopic methods. One such method would be the development of electrochemical-muon spectroscopy techniques in order to produce novel reactive intermediates electrochemically, or using a combination of electrochemical methods followed by muon irradiation. We will then investigate the electronic structure of these reactive intermediates through the coupling of nuclei to unpaired electrons (hyperfine interactions) by muon methods. I will continue to use the interdisciplinary setting and state-of-the-art experimental tools at the two major facilities that we use, TRIUMF national laboratory in Vancouver, Canada, and Rutherford Appleton laboratory in the UK, combined with the computational chemistry methods and conventional lab methods to provide a unique training environment for undergraduate and Master students involved in this research program. For our research on supercritical fluids and ionic liquids, we will focus on providing mechanistic and dynamics information related to free radical chemistry and intermolecular interactions that are relevant to potential chemical and manufacturing industries.