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

我们希望在室温离子液体和亚超临界流体中进行化学动力学研究。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，我们将能够为基于超临界流体的工艺或基于离子液体的工艺中的离子液体类型找到最佳热力学条件。在我们的许多研究中，我们使用了μ子，从化学的角度来看，μ子可以被认为是轻质子。我们还想扩展一种新的技术，激光泵浦μ子探测技术，我们最近开发的研究在激发态的原子氢反应的动力学同位素效应，探测电离辐射过程中的瞬态，以及自由基的激发态中间体。我们还希望开发其他新的光谱方法。一种这样的方法将是电化学μ子光谱技术的发展，以产生新的活性中间体电化学，或使用电化学方法的组合，然后μ子照射。然后，我们将研究这些活性中间体的电子结构，通过耦合的核未成对电子（超精细相互作用）的μ子方法。我将继续使用跨学科的设置和国家的最先进的实验工具，在我们使用的两个主要设施，TRIUMF国家实验室在温哥华，加拿大，和卢瑟福阿普尔顿实验室在英国，结合计算化学方法和传统的实验室方法，提供一个独特的培训环境，本科生和硕士生参与本研究计划。对于我们对超临界流体和离子液体的研究，我们将专注于提供与潜在的化学和制造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.