Dynamic control and self-assembly of ortho-phenylene foldamers

有了这个奖项，化学系的大分子、超分子和纳米化学项目将资助C。来自迈阿密大学的斯科特·哈特利开发了能够复制并最终补充天然大分子的非凡能力的分子。 很长一段时间以来，合成化学家一直在努力制备与蛋白质和核酸大小和复杂性相当的分子。 人体需要20秒到几分钟来制造蛋白质。 相比之下，将数百种氨基酸制备和组装成同一蛋白质的长链需要化学家几天到几个月的时间，如果可能的话。此外，基于生物化学构建模块设计新的结构复杂的系统是极具挑战性的。 该项目通过利用更小和更容易制备的分子的组装来避免繁琐的合成路径。该奖项的结果预计将提供有关结构复杂分子之间的性质，动力学和相互作用的基本答案，这与开发具有与大型生物分子相似能力的人工系统有关。 虽然目标化合物在化学上不一定等同于生物大分子，但它们在折叠和识别等相关过程中的行为是相似的。 更广泛的影响，这项工作包括实验室模块的发展，介绍有机化学课程，本科生参与研究，并参与了一个联盟的俄亥俄州大学，旨在支持代表性不足的少数民族学生在STEM领域。这项工作的重点是调查的动态控制和自组装邻亚苯基foldamers。 在开发这些折叠体的过程中，生物大分子的能力，如分子识别、催化和响应行为（分子“机械”），可以潜在地被复制，从而通过简单和非繁琐的分子设计提供对复杂过程的访问。 为了实现这一目标，进行了几项研究，涉及氟化邻苯的发展，控制动态系统与可切换的扭曲和远程构象通信，以及扭曲大环组装的结构-性能效应。 氟核磁共振光谱的使用是特别有趣的，因为这种技术是简单的，但提供了一个有影响力的方法来阐明这些邻亚苯基系统的折叠行为。 从概念上讲，这项工作有望在折叠体领域、构象动力学和复杂结构的合成方面提供基本答案。该奖项反映了NSF的法定使命，并被认为值得通过使用基金会的智力价值和更广泛的影响审查标准进行评估来支持。

With this award, the Macromolecular, Supramolecular, and Nanochemistry Program in the Division of Chemistry is funding Dr. C. Scott Hartley from Miami University to develop molecules that replicate and ultimately complement the remarkable capabilities of naturally occurring macromolecules. For a very long time, synthetic chemists have struggled to prepare molecules of comparable size and complexity to proteins and nucleic acids. It takes the human body anywhere between 20 seconds to a couple of minutes to make a protein. In contrast, preparing and assembling hundreds of amino acids into a long chain of the same protein would take a chemist days to months, if it is even possible at all. Further, designing new structurally-complex systems based on biochemical building blocks is extremely challenging. This project avoids tedious synthetic paths by taking advantage of the assembly of smaller and more-easily prepared molecules. The results from this award are expected to provide fundamental answers about the nature, dynamics and interactions between structurally complex molecules, which are of relevance to developing artificial systems with similar capabilities to large biological molecules. While the target compounds are not necessarily chemically equivalent to biomacromolecules, their behavior in relevant processes such as folding and recognition is similar. The broader impacts of this work include the development of laboratory modules for introductory organic chemistry courses, undergraduate involvement in research, and participation in a consortium of Ohio universities aimed at supporting underrepresented minority students in the STEM fields.This work is focused on the investigation of the dynamic control and self-assembly of ortho-phenylene foldamers. In developing these foldamers, the capabilities of biomacromolecules, such as molecular recognition, catalysis, and responsive behavior (molecular "machinery"), can potentially be replicated, providing access to complex processes through simple and non-tedious molecular design. Several studies are carried out in order to achieve this goal, involving the development of fluorinated o-phenylenes, controlling dynamic systems with switchable twist and long-range conformational communication, and structure-property effects for the assembly of twisted macrocycles. The use of fluorine nuclear magnetic resonance spectroscopy is particularly interesting because this technique is simple and yet offers an impactful method for elucidating the folding behavior of these ortho-phenylene systems. Conceptually, this work is expected to provide fundamental answers in the context of the foldamer field, conformational dynamics, and the synthesis of complex structures.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.