Dynamic metallo-supramolecular oligomers stabilized by Cucurbit[8]uril connectors: self-assembly applied to combinatorial chemistry

Cucurbit[8]uril 连接器稳定的动态金属超分子低聚物：自组装应用于组合化学

• 批准号: 1507321
• 负责人: Eric Masson
• 金额: $ 43.5万
• 依托单位: Ohio University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2015
• 资助国家: 美国
• 起止时间: 2015-06-01 至 2019-12-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1507321&HistoricalAwards=false
• 关键词: Dynamic; metallo; supramolecular; oligomers; stabilized; Dynamic; metallo; supramolecular; oligomers; stabilized

With the support of the Macromolecular, Supramolecular and Nanochemistry (MSN) program of the NSF Division of Chemistry, Prof. Masson investigates the recognition properties of water soluble metal-ligand complexes towards CB[n] and develops dynamic combinatorial approaches to preparing dynamic oligomers and polymers. Synthetic polymers are found in most objects used in everyday life. Polymers that spontaneously adjust their composition depending on their environment in water are of particular interest to Professor Eric Masson at Ohio University. His research group studies the formation and properties of a novel type of dynamic polymers in which the interchangeable building blocks are tied to one another with a pumpkin-shaped, hollow molecular ring called cucurbit[8]uril (CB[8]). The project has potential applications in biochemistry, as the dynamic polymers can interact with medically or biologically relevant materials such as proteins and cells, and in analytical chemistry, as the polymers can be used as sensors in quality control and drug detection applications. This project is multidisciplinary, and provides training to undergraduate and graduate students with a broad range of interests and talents, from organic synthesis, to biochemistry and statistical analysis. In addition, students are involved in the upgrade of an organic synthesis board game created by Professor Masson for computer tablets. The building blocks of the dynamic oligomers targeted herein are metal-terpyridine complexes linked to CB[8]-binding units. The terpyridine ligands bear phenyl or naphthyl groups at the 4'-position to promote binding in the CB[8] ring. The terpyridine ligands are also functionalized with bio-inspired side chains (based mostly on amino acid residues) at the 4- and 4"-positions for interactions with the outer wall of CB[8] and for target recognition. The metal-ligand complexes are connected non-covalently via binding to the CB[8] rings. The outer wall of CB[8] participates de facto in the target recognition process once the metal-ligand/CB[8] oligomers are formed. This project involves (1) the preparation of a library of metal-ligand complexes (such as iron(II)-, ruthenium(II)- and iridium(III)-terpyridine) with a variety of pendent groups; (2) the assessment of their recognition properties towards CB[n]s and the interactions between the pendent groups with the outer convex surface of CB[n]s; and (3) the preparation and characterization of the metal-ligand/CB[8] dynamic oligomers in the absence and presence of biologically relevant targets.

在NSF化学划分的大分子，超分子和纳米化学（MSN）计划的支持下，Masson教授调查了水溶性金属配体配合物对CB [n]的识别性能，并开发了动态组合方法，以制备动态寡聚物和聚合物。在日常生活中使用的大多数对象中都发现了合成聚合物。俄亥俄州大学的埃里克·马森教授特别感兴趣的是自发地调整其成分的聚合物。他的研究小组研究了一种新型的动态聚合物的形成和特性，其中可互换的构建块与南瓜形的空心分子环相互绑定，称为Cucurbit [8]尿液（CB [8]）。该项目在生物化学中具有潜在的应用，因为动态聚合物可以与医学或生物学相关的材料（例如蛋白质和细胞）以及分析化学相互作用，因为聚合物可以用作质量控制和药物检测应用中的传感器。该项目是多学科的，并为本科生和研究生提供了广泛的兴趣和才能的培训，从有机综合到生物化学和统计分析。此外，学生还参与了Masson教授为计算机平板电脑创建的有机合成棋盘游戏的升级。本文靶向的动态寡聚物的构件是与CB相关的金属 - 甲吡啶络合物[8]结合单元。 甲吡吡啶配体在4'位置携带苯基或萘基，以促进Cb中的结合[8]环。 在4和4“和4”位置与CB的外壁相互作用，以及用于目标识别的4英寸和4英寸的位置，以及金属 - 辅助配合物通过与CB [8]的靶向识别，CB [8] Rings de 8]，terpyridine配体还通过生物启发的侧链（主要基于氨基酸残基）功能化。形成金属 - 配体/CB [8]寡头。 CB [N] S;（3）在没有生物学相关的目标的情况下，金属配体/CB的制备和表征。