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，极大地影响了我们在分子水平上对物质的理解。使用这些方法，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特性、它们内部的转变和反应。该提案重点关注两个关键领域，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且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、气体水合物和金属有机骨架材料如何以及何时形成等的基本理解。它还可能最终带来抑制天然气水合物堵塞管道或控制与羟基自由基有关的疾病（例如癌症和衰老）的新方法。这项研究的结果具有广泛影响的潜力，例如可以改善医疗保健结果、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巨大储量中的巨大能源财富。 ***我们的工作将继续巩固我们在多个领域使用分子模拟的既定领导地位，这些领域目前看来可能取得重大进展。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的基础上，将探讨分子排列及其动力学，以表征关键结构和事件及其在其中的作用这些订购流程。气体笼形水合物、冰和金属有机骨架（MOF）这些具有广泛兴趣和重要性的材料将是我们关注的主要焦点。我们最近扩展到并取得重大进展的另一个具有挑战性的领域是凝聚相中羟基自由基 (OH*) 的分子模拟。我们将探索各种水环境（例如水或冰内部或表面）中这种关键化学物质的局部结构及其影响，其中我们将探讨 OH* 与各种小分子的相互作用和反应，这些小分子对于大气和生化背景。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，使我们能够从所执行的模拟中获得额外的见解（超出目前可用的见解），从而使我们对这些系统和流程的理解取得重大进展。 **