Exploration of Active Roles of Water in Aqueous Supramolecular Chemistry

水在水性超分子化学中的活性作用探索

• 批准号: RGPIN-2021-03245
• 负责人: Wang, Xiaosong
• 金额: $ 2.11万
• 依托单位: University of Waterloo
• 依托单位国家: 加拿大
• 项目类别: Discovery Grants Program - Individual
• 财政年份: 2022
• 资助国家: 加拿大
• 起止时间: 2022-01-01 至 2023-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=748148
• 关键词: Exploration; Active; Roles; Water; Aqueous

Hydrophobic effect-caused self-assembly (HE-SA) is conventionally defaulted as a process of hydrophobic interaction (HI) of non-polar groups. This default is one reason for the perplexity of HE-SA behavior in many cases, including biological systems, because the roles of water are neglected. Computer simulations have proposed that HEs stem from the free energy of water structure (dynamic hydrogen bonding network). The water structures are different between bulk water and the water hydrating hydrophobic molecules, known as hydrophobic hydration (HH), which cause an energy difference driving HE-SA. Consequently, the HH water is either repelled to gain entropy (conventional HE-SA) or reserved to act as an assembling component involved within the assemblies via an enthalpy/entropy compensation. The latter scenario is commonly observed in biological systems and the water component is responsible for the functions, which is the inspiration and motivation to advance the conventional HE-SA. The goal of my research is to experimentally understand the role of water in the construction and function of self-assembled colloids, which will promote supramolecular synthesis for water-mediated functions and industrial innovation of aqueous materials and technologies. My team and I have (1) explored the synthesis and aqueous self-assembly of water-insoluble metal carbonyl compounds with various structures, (2) discovered the first aqueous assembly without HI, which involves water as a major assembling component and (3) developed a number of practical techniques for water characterizations. Building on this progress, the proposed research program will target three objectives towards the comprehensive knowledge of HE-SA: (O1) Examine the possibility to transfer the knowledge already learned from the metal carbonyl organometallic to organic systems, which is essential to promote extensive studies to advance HE-SA; (O2) Explore the water component within the discovered organometallic assembly to learn its role in the construction of functional colloids; (O3) Elucidate water behavior in the HE-SA in relation to the chemical structure of the organometallic building blocks, including small molecules, linear and cyclic macromolecules. The research will advance the conventional knowledge of HE-SA and create a new niche to explore water-mediated functions for self-assembled colloids, which will promote Canada's position in research internationally, strengthen the R & D capacity for the innovation of aqueous biomedical, agricultural and household products, etc. and thus contribute to Canada's pillar industries. The students will be trained in relevant technical skills, research interests and, particularly, scientific vision, so they will be expected to take a leadership role after the training to further advance the field, create high tech jobs and establish Canada as an innovation hub.

疏水效应引起的自组装（HE-SA）通常被默认为非极性基团的疏水相互作用（HI）过程。这种默认是 HE-SA 在许多情况下（包括生物系统）行为混乱的原因之一，因为水的作用被忽视了。计算机模拟提出 HE 源于水结构的自由能（动态氢键网络）。本体水和水合疏水分子之间的水结构不同，称为疏水水合（HH），这会导致驱动 HE-SA 的能量差异。因此，HH 水要么被排斥以获得熵（传统的 HE-SA），要么被保留作为通过熵/熵补偿参与组件内的组装组件。后一种情况在生物系统中很常见，而水成分负责其功能，这是推进传统HE-SA的灵感和动力。我的研究目标是通过实验了解水在自组装胶体的构建和功能中的作用，这将促进水介导功能的超分子合成以及水性材料和技术的工业创新。我和我的团队 (1) 探索了具有各种结构的水不溶性金属羰基化合物的合成和水自组装，(2) 发现了第一个不含 HI 的水组装，其中水作为主要组装成分，(3)开发了许多用于水表征的实用技术。在此进展的基础上，拟议的研究计划将针对 HE-SA 综合知识的三个目标：（O1）审查将已从金属羰基有机金属学到的知识转移到有机系统的可能性，这对于促进广泛的研究至关重要推进HE-SA； (O2) 探索所发现的有机金属组装体中的水成分，以了解其在功能胶体构建中的作用； (O3) 阐明 HE-SA 中的水行为与有机金属构件（包括小分子、线性和环状大分子）化学结构的关系。该研究将推进HE-SA的常规知识，并创造一个新的领域来探索自组装胶体的水介导功能，这将提升加拿大在国际研究中的地位，增强水性生物医学创新的研发能力，农产品、家居产品等，为加拿大的支柱产业做出了贡献。学生将接受相关技术技能、研究兴趣，特别是科学视野方面的培训，因此他们将在培训后发挥领导作用，进一步推进该领域的发展，创造高科技就业机会，并将加拿大打造成创新中心。