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Reactive Scattering Dynamics at the Gas-Liquid Interface: Bridging the Gap between the Gas-Phase and Solution

气液界面的反应散射动力学：弥合气相和溶液之间的间隙

基本信息

批准号：
EP/M021823/1
负责人：
Matthew Costen
金额：
$ 103.02万
依托单位：
Heriot-Watt University
依托单位国家：
英国
项目类别：
Research Grant
财政年份：
2015
资助国家：
英国
起止时间：
2015 至无数据
项目状态：
已结题

来源：
https://gtr.ukri.org/projects?ref=EP%2FM021823%2F1
关键词：
Reactive Scattering Dynamics Gas Liquid

项目摘要

Anywhere the gas and liquid phases meet, chemistry occurs at the interface. Examples in the natural world include: respiration in living organisms; atmospheric aerosol particles; the surface of the sea on Earth; hydrocarbon particles in the atmosphere of Saturn's moon Titan. The chemistry of these interfaces is also vital in man-made environments as well: combustion of liquid fuels; industrial processes such as multiphase catalysis, gas sequestration and distillation. However, despite their importance, in comparison to the chemistry of reactions in the gas-phase or in solution, reactions at the gas-liquid interface are much less well understood. This project aims to deepen our fundamental understanding of reactions at liquid surfaces through a combination of cutting-edge experiment and theory. Consider a gas molecule approaching a liquid surface. The first encounter it makes with the surface will be an isolated event; the gas phase molecule will collide with a single molecule of the liquid surface. At this point the encounter is essentially the same as a gas phase collision between two isolated molecules. In the gas-phase, the molecules will then recoil and the encounter will be over. In some cases, collisions at the liquid surface will also result in the gas-phase molecule rebounding back into the gas-phase. However, it may instead go on to collide with further liquid surface molecules, and may even pass through the surface of the liquid and into solution, before eventually returning to the gas-phase. Reactions at the gas-liquid interface thus share characteristics of both the gas and solution phases, and by studying the dynamics of the reactions we can bridge the gap between them. This complements the intensive on-going effort in these hitherto largely separate areas, providing a unifying picture of molecular scattering dynamics. We will develop a new apparatus for our experiments, based on our previous experience in gas-liquid interfacial scattering, and combine it with high-resolution laser spectroscopy previously applied to study gas-phase dynamics. We will use this to study the reaction of CN radicals with liquid hydrocarbons, which forms HCN. The dynamics of this benchmark reaction process have been previously studied in the gas and solution phases. This reaction is not only of fundamental interest, as the CN radical is an important reactive species in extra-terrestrial atmospheres (e.g. atmosphere of Titan), and liquid hydrocarbon combustion. Simultaneously with the experiments, we will develop new theoretical models of the forces between the atoms present, and use those in calculations to simulate the dynamics of the reactions under experimental conditions. We will compare and combine the results of the experiments and theory to provide the most-detailed ever description of gas-liquid interfacial reaction dynamics. The fundamental insights into dynamics at the gas-liquid interface provided by this work will inform our understanding and modelling of the processes at gas-liquid interfaces in a wide range of environments vital to our society, e.g. atmospheric aerosols, liquid fuel combustion.

在气相和液相相遇的任何地方，化学反应都会在界面处发生。自然界中的例子包括：生物体的呼吸；大气气溶胶颗粒；地球上的海洋表面；土星卫星泰坦大气中的碳氢化合物颗粒。这些界面的化学性质在人造环境中也至关重要：液体燃料的燃烧；工业过程，如多相催化、气体封存和蒸馏。然而，尽管气液界面的反应很重要，但与气相或溶液中的反应化学相比，人们对气液界面反应的了解却要少得多。该项目旨在通过尖端实验和理论的结合，加深我们对液体表面反应的基本理解。考虑接近液体表面的气体分子。它与表面的第一次接触将是一个孤立的事件；气相分子将与液体表面的单个分子碰撞。此时的相遇本质上与两个孤立分子之间的气相碰撞相同。在气相中，分子将反冲，相遇就会结束。在某些情况下，液体表面的碰撞也会导致气相分子反弹回气相。然而，它可能会继续与进一步的液体表面分子碰撞，甚至可能穿过液体表面并进入溶液，然后最终返回气相。因此，气液界面的反应具有气相和溶液相的特征，通过研究反应动力学，我们可以弥补它们之间的差距。这补充了这些迄今为止基本上独立的领域正在进行的大量努力，提供了分子散射动力学的统一图像。我们将根据我们之前在气液界面散射方面的经验，为我们的实验开发一种新设备，并将其与之前用于研究气相动力学的高分辨率激光光谱相结合。我们将用它来研究 CN 自由基与液态烃的反应，形成 HCN。先前已在气相和溶液相中研究了该基准反应过程的动力学。该反应不仅具有根本意义，因为 CN 自由基是地外大气（例如泰坦大气）和液态烃燃烧中的重要反应物种。在进行实验的同时，我们将开发原子之间力的新理论模型，并在计算中使用这些模型来模拟实验条件下反应的动力学。我们将比较并结合实验和理论的结果，以提供气液界面反应动力学最详细的描述。这项工作提供的对气液界面动力学的基本见解将有助于我们理解和建模对我们社会至关重要的各种环境中的气液界面过程，例如，环境。大气气溶胶、液体燃料燃烧。