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.**

分子模拟已成为非常强大的工具，这些工具正在极大地影响我们对分子水平的物质的理解。使用这种方法，我们可以检查分子相互作用并发展的分子集合，从而提供新的科学见解。我的研究的总体目的是探究液体和固体系统的微观行为，以进一步了解它们对它们的各种化学和物理特性，它们内部的转化和反应。该提案的重点是两个关键领域，一个旨在探索重要材料类别的结晶和订购过程，另一个旨在在各种水性环境中研究关键和高度反应性化学物种的行为，即羟基自由基的行为。这项工作将提高我们对冰，气体水合和金属有机框架材料的基本理解，例如如何以及何时形成。它最终也可能导致抑制管道中气体水合物塞的新方法或控制与羟基自由基（例如癌症和衰老）链接的疾病。这项研究的结果通过导致改善医疗保健结果，更有效和有效的废水处理，更好的气候模型提供改善的天气预测，并获得目前存储在大量天然气水合物中的巨大能源储备。成核和晶体形成和生长的基础的过程将是我们研究的重点，基于我们的专业知识和经验，在这些领域中，将探测分子排列及其动力学，以表征关键结构和事件及其在这些顺序过程中的作用。气体覆盖水合物，冰和金属有机框架（MOF）是广泛关注和重要性的材料，将是我们关注的主要重点。我们最近已经扩展到了另一个具有挑战性的领域，并在凝结相中对羟基自由基（OH*）的分子模拟进行了重大进步。将探索各种水性环境中该关键化学物种的局部结构及其影响，例如在内部或水面，水或冰的表面），我们将在其中探测OH*与对大气和生化环境重要的各种小分子的相互作用和反应。多尺度建模方法将是本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，使我们能够从进行的模拟中获得其他见解（超出当前可用的见解），从而使我们对这些系统和流程的理解有了重大的进步。**