Gas Phase Supramolecular Characterization

气相超分子表征

• 批准号: 0957757
• 负责人: David Dearden
• 金额: $ 23.5万
• 依托单位: Brigham Young University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2010
• 资助国家: 美国
• 起止时间: 2010-06-01 至 2013-05-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=0957757&HistoricalAwards=false
• 关键词: Gas; Phase; Supramolecular; Characterization

With support from the Chemical Measurement and Imaging program, Prof. David Dearden and his group at Brigham Young University are devising new approaches to the detection and characterization of prototypical molecular devices based on pumpkin-shaped molecules (named cucurbiturils, after the Latin name for "pumpkin") that constitute some of the smallest possible containers. The methods being developed complement existing techniques by providing better sensitivity. They include the first infrared multiphoton dissociation studies of these materials, essentially using infrared laser light to take "snapshots" that reveal the way the devices fit together. Cucurbiturils and related "containers" are being investigated in other laboratories for potential applications in such diverse areas as components of molecular machines; in drug encapsulation, protection, and delivery; and in sensitive new analytical assays such as the direct detection of insulin levels in the blood (relevant to the detection and treatment of diabetes). It is widely recognized that the binding properties of cucurbiturils are sensitively dependent on solvents and counterions, yet the reasons for this dependence are not clearly understood. Hence, these fundamental gas-phase studies of structures in the absence of solvent and counterions are vital to gain understanding needed to facilitate future applications, addressing questions such as how trapping molecules inside the cavity affects the binding of cations on the rims, the mechanism of exchange of bound/trapped species, and the origin of the large shifts in acidity that occur for trapped guests.The characterization methods being developed will enable applications of this "supramolecular" chemistry that may ultimately impact manufacturing, computing, and medicine. The techniques will also be immediately useful to biomolecular studies involving nature's "molecular machines," proteins. The work will also have important educational benefits. Graduate students will be trained in advanced techniques for high performance mass spectrometry that are vital for the biotechnology industry and the emerging field of proteomics. A parallel aim is to attract talented undergraduate students to chemical research. Toward this aim, the instrumentation supported is also used in undergraduate courses in analytical and physical chemistry, providing direct experience with advanced techniques most students would not otherwise see outside of graduate school.

在化学测量和成像项目的支持下，杨百翰大学的大卫·迪尔登教授和他的团队正在设计新的方法来检测和表征基于南瓜形状分子的原型分子器件（以“南瓜”的拉丁名称命名为葫芦脲），这些分子构成了一些最小的容器。 正在开发的方法通过提供更好的灵敏度来补充现有技术。 它们包括对这些材料的第一次红外多光子解离研究，基本上是使用红外激光来拍摄“快照”，以揭示这些设备组装在一起的方式。 葫芦脲和相关的“容器”正在其他实验室进行研究，以在分子机器的组件等不同领域的潜在应用;在药物封装，保护和交付;和在敏感的新的分析测定，如直接检测血液中的胰岛素水平（相关的检测和治疗糖尿病）。人们普遍认为，葫芦脲的结合特性敏感地依赖于溶剂和抗衡离子，但这种依赖性的原因还不清楚。因此，在没有溶剂和抗衡离子的情况下，这些基本的气相结构研究对于获得促进未来应用所需的理解至关重要，解决诸如腔体内的捕获分子如何影响边缘上阳离子的结合，结合/捕获物质的交换机制，和捕获的客人发生的酸度大的变化的起源。正在开发的表征方法将使这种“超分子”的应用化学可能最终影响制造业，计算和医学。这些技术也将立即用于涉及自然界“分子机器”蛋白质的生物分子研究。 这项工作也将有重要的教育效益。研究生将接受高性能质谱的先进技术培训，这些技术对生物技术行业和新兴的蛋白质组学领域至关重要。一个平行的目标是吸引有才华的本科生从事化学研究。为了实现这一目标，支持的仪器也被用于分析和物理化学的本科课程，提供先进技术的直接经验，否则大多数学生不会看到研究生院之外。