The behaviour of OH* in aqueous environments, nucleation of gas hydrates, and ordering processes in MOFs: insights from molecular simulations

分子模拟已经成为非常强大的工具，极大地影响了我们在分子水平上对物质的理解。使用这种方法，我们可以检查相互作用和进化的分子集合，从而提供新的科学见解。我研究的总体目标是探索液体和固体系统的微观行为，以进一步了解它们的各种化学和物理性质，它们在其中的转化和反应。该提案侧重于两个关键领域，一个旨在探索重要材料类别的结晶和排序过程，另一个集中于研究一个关键和高活性化学物质羟基自由基在各种水环境中的行为。这项工作将提高我们对冰、天然气水合物和金属有机框架材料如何以及何时形成的基本理解。它还可能最终导致新的方法来抑制管道中的天然气水合物堵塞，或控制与羟基自由基有关的疾病，如癌症和衰老。这项研究的结果有可能产生广泛的影响，例如，可以改善医疗保健结果，提高废水处理的效率和效果，改进气候模型，提供更好的天气预报，以及利用目前储存在大量天然气水合物中的巨大能源财富。

Molecular simulations have become very powerful tools that are dramatically impacting our understanding of matter at the molecular level. Using such approaches, we can examine collections of molecules interacting and evolving thereby providing new scientific insights. The overall aim of my research is to probe the microscopic behaviour of liquid and solid systems in order to further our understanding of their various chemical and physical properties, their transformations and reactions within them. This proposal focuses on two key areas, one aimed at exploring crystallization and ordering processes for important classes of materials, and the other centered on investigating the behaviour of a key and highly reactive chemical species, the hydroxyl radical, in various aqueous environments. This work will improve our fundamental understanding of, for example, how and when ice, gas hydrates and metal-organic framework materials may form. It may also eventually lead to new ways to inhibit gas hydrate plugs in pipelines or to control diseases that have links to the hydroxyl radical, such as cancer and aging. The results of this research have potential for broad impact by leading to, for example, improved health-care outcomes, more efficient and effective wastewater treatments, better climate models providing improved weather forecasts, and access to the enormous energy wealth currently stored in vast reserves of natural gas hydrates. Our work will continue to build on our established leadership in using molecular simulations in several areas, where significant advances now appear possible. Nucleation and the processes underlying the formation and growth of crystals will remain an area of focus of our research, building upon our expertise and experience, where molecular arrangement and their dynamics will be probed in order to characterize key structures and events, and their roles within these ordering processes. Gas clathrate hydrates, ice and metal-organic frameworks (MOFs), materials of broad interest and importance, will be primary focuses of our attention. Another challenging area we have recently expanded into, and made significant advances within, is the molecular simulations of the hydroxyl radical (OH*) in condensed phases. The local structure and its impacts for this key chemical species in various aqueous environments (e.g. within, or on the surfaces of, water or ice) will be explored, where we will probe the interactions and reactions of OH* with various small molecules important to atmospheric and biochemical contexts. Multiscale modeling approaches will be a common theme across many aspects of this work. We will continue to pioneer new analysis and visualization tools to allow us to gain additional insights (beyond those currently available) from the simulations performed, thereby allowing for significant advances to our understanding of these systems and processes.