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

OH* 在水环境中的行为、气体水合物的成核以及 MOF 中的有序过程：来自分子模拟的见解

• 批准号: RGPIN-2016-03845
• 负责人: Kusalik, Peter
• 金额: $ 3.35万
• 依托单位: University of Calgary
• 依托单位国家: 加拿大
• 项目类别: Discovery Grants Program - Individual
• 财政年份: 2018
• 资助国家: 加拿大
• 起止时间: 2018-01-01 至 2019-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=656161
• 关键词: behaviour; OH; aqueous; environments; nucleation

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.**

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。***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既定领导地位上，这些领域现在可能取得重大进展。在我们的专业知识和经验的基础上，成核和晶体形成和生长的过程将继续是我们研究的重点领域，在这里，分子排列和它们的动力学将被探索，以表征关键结构和事件，以及它们在这些排序过程中的作用。气体包合水合物、冰和金属有机框架（mof）等具有广泛意义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，是缩合相中羟基自由基（OH*）的分子模拟。在不同的水环境中（例如，在水或冰的内部或表面），我们将探索这种关键化学物质的局部结构及其影响，在那里我们将探索OH*与各种对大气和生化环境重要的小分子的相互作用和反应。多尺度建模方法将成为这项工作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，使我们能够从模拟中获得更多的见解（超出目前可用的），从而使我们对这些系统和过程的理解取得重大进展