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，我们可以研究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，一个旨在探索重要类别材料的结晶和有序过程，另一个集中于研究关键和高活性化学物质羟基自由基在各种水性环境中的行为。这项工作将提高我们对冰、天然气水合物和金属有机骨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气体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，改善医疗保健结果，更高效和有效的废水处理，更好的气候模型提供更好的天气预报，以及获得目前储存在天然气水合物储量中的巨大能源财富。我们的工作将继续建立在我们在几个领域使用分子模拟的领导地位上，这些领域现在似乎有可能取得重大进展。成核和晶体形成和生长的过程将仍然是我们研究的重点领域，建立在我们的专业知识和经验基础上，分子排列及其动力学将被探索，以表征关键结构和事件，以及它们在这些有序过程中的作用。气体笼形水合物、冰和金属有机骨架（MOFs）等具有广泛兴趣和重要性的材料将是我们关注的主要焦点。我们最近扩展到的另一个具有挑战性的领域，并取得了重大进展，是凝聚相中羟基自由基（OH*）的分子模拟。将探索这种关键化学物质在各种水性环境中的局部结构及其影响（例如，在水或冰的表面上），我们将探索OH* 与各种小分子的相互作用和反应，这些小分子对大气和生物化学环境很重要。多尺度建模方法将是这项工作的许多方面的共同主题。我们将继续开拓新的分析和可视化工具，使我们能够从所执行的模拟中获得更多的见解（超出目前可用的见解），从而使我们对这些系统和过程的理解取得重大进展。

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.**