Dynamics of Small Molecules in Supramolecular Systems

超分子系统中小分子的动力学

• 批准号: 121389-2012
• 负责人: Bohne, Cornelia
• 金额: $ 5.1万
• 依托单位: University of Victoria
• 依托单位国家: 加拿大
• 项目类别: Discovery Grants Program - Individual
• 财政年份: 2015
• 资助国家: 加拿大
• 起止时间: 2015-01-01 至 2016-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=569184
• 关键词: Dynamics; Small; Molecules; Supramolecular; Systems

Supramolecular systems form reversibly from molecular building blocks. My research focuses on understanding the dynamics of supramolecular systems. I have a strong track record in methodology development, and mechanistic understanding is gained from extensive structure-dynamics relationship studies. The fundamental knowledge obtained has impact on how functional supramolecular systems are employed and will aid others in the rational design of functional systems, such as drug delivery, catalysis and sensing. The proposed work focuses on host systems with varying degrees of complexity, ranging from highly dynamic supramolecular aggregates (bile salts), to complex molecular environments (proteins), to simple molecular systems (cucurbit[n]urils). - Bile salt aggregates have different binding sites. Structure-dynamics studies will be extended to investigate intra-aggregate mobility at high guest loading. A new direction will take studies from solution to confined spaces in gels since many of the applications of supramolecular systems will require confinement on surfaces or solids. - Proteins bind guests in multiple sites with very different affinities. We showed that the desired reactivity for a bimolecular reaction was highest when the reagents were bound to protein sites with moderate affinity, which is not the generally expected trend. Photophysical techniques will be applied to specifically address reagents in the most reactive sites. New methodologies are required because traditional techniques, such as X-Ray crystallography, do not provide information on the reagents bound to moderate affinity sites. - Cucurbit[n]urils are hosts that bind guests with very high binding constants, which rival those observed for biological systems. The reasons for these high binding constants are not fully understood. Dynamic information on the guest binding to cucurbit[n]urils is currently limited. Structure-dynamics relationship studies are proposed to provide a comprehensive mechanistic understanding on guest@cucurbit[n]uril systems.

超分子系统从分子构建块可逆地形成。我的研究重点是了解超分子系统的动态。我在方法论开发方面有很强的记录，并且从广泛的结构障碍关系研究中获得了机理理解。获得的基本知识会影响功能性超分子系统的使用方式，并将帮助其他人进行功能系统的合理设计，例如药物输送，催化和感应。 所提出的工作集中于具有不同程度复杂性的宿主系统，范围从高度动态的超分子骨料（胆汁盐）到复杂的分子环境（蛋白质）到简单的分子系统（cucurbit [n]尿液）。 - 胆汁盐骨料具有不同的结合位点。结构动力学研究将进行扩展，以调查高客人负荷下聚集的迁移率。一个新的方向将研究从溶液到凝胶中的密闭空间，因为超分子系统的许多应用都需要在表面或固体上限制。 - 蛋白质在具有非常不同亲和力的多个站点的客人结合。我们表明，当试剂与中等亲和力的蛋白质位点结合时，双分子反应的所需反应性最高，这不是普遍期望的趋势。光物理技术将应用于最具反应性位点中的特异性试剂。需要新的方法，因为传统技术（例如X射线晶体学）不提供有关与中等亲和力位点的试剂的信息。 -Cucurbit [n]尿液是宿主，它们具有很高的结合常数，它们与生物系统观察到的宿主相媲美。这些高结合常数的原因尚未完全理解。目前，有关客人与墨西哥犬[N]尿路的绑定的动态信息受到限制。提出了结构动力学关系研究，以对访客@cucurbit [n]尿液系统提供全面的机械理解。