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

我们想要研究室温离子液体以及亚临界和超临界流体中的化学动力学。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液体，没有明显的气相和液体相。从长远来看，我们的研究将为我们提供有用的信息，有助于设计既经济又环保的新型工业工艺。特别是，我们将能够为基于超临界流体的过程或基于离子液体的过程中的离子液体类型找到最佳的热力学条件。在我们的许多研究中，我们使用的是介子，从化学的观点来看，它可以被认为是轻质子。我们还想扩展我们最近发展起来的一种新技术，激光泵浦缪子探测技术，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变，以及激发态中的自由基中间体。我们还想开发其他新的光谱方法。其中一种方法是开发电化学-Muon光谱技术，以便通过电化学方法产生新的活性中间体，或者使用电化学方法的组合，然后再进行Muon辐射。然后，我们将用Muon方法通过核与未配对电子的耦合(超精细相互作用)来研究这些活性中间体的电子结构。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实验室方法，为参与本研究项目的本科生和硕士学生提供独特的培训环境。在我们对超临界流体和离子液体的研究中，我们将专注于提供与潜在的化学和制造行业相关的自由基化学和分子间相互作用的机理和动力学信息。

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.