Novel Synthetic Methods

新的合成方法

• 批准号: 2246075
• 负责人: Vladimir Gevorgyan
• 金额: $ 49.6万
• 依托单位: University of Texas at Dallas
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2023
• 资助国家: 美国
• 起止时间: 2023-08-01 至 2026-07-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2246075&HistoricalAwards=false
• 关键词: Novel; Synthetic; Methods

With the support of the Chemical Synthesis Program in the Division of Chemistry, Professor Vladimir Gevorgyan and his graduate and undergraduate students at the University of Texas at Dallas are developing mild, efficient, and selective reaction methodology for synthesizing organic molecules. In particular, the Gevorgyan group is developing organic chemistry methodology to convert readily available feedstock chemicals that have an abundance of Carbon–Hydrogen (C–H) bonds into other, more highly valued chemicals that contain new bonds that are more commonly found in medicines and materials (Carbon–Oxygen (C–O), Carbon–Nitrogen (C–N), Carbon–halogen (C–X), Carbon–Carbon (C–C), Carbon–Boron (C–B), etc.). To carry out these transformations, Professor Gevorgyan’s team is developing reaction methodology that is free of costly and potentially toxic and/or explosive reagents. In addition to providing new and effective routes to building complex molecules and materials of importance, the broader impacts of the proposed work include outreach activities that are aimed at recruiting undergraduate students, including underrepresented minority students, into research where their potential and career possibilities will be enhanced.In this project, the Gevorgyan team is developing new mild methods for the generation of carbon- and heteroatom-centered radicals and unlocking their reactivity. The approach under development relies on novel donor-acceptor (DA) complexes capable of the reduction of electrophilic intermediates using single electron transfer (SET). Their work is being carried out using visible light initiation leading to the generation of a precursor radical that undergoes atom transfer (AT) or hydrogen atom transfer (HAT) to generate transposed radicals. These new radicals can then engage in a number of diverse synthetic transformations, including C(sp3)−H bond functionalization reactions. The factors favoring the efficient formation of DA complexes, as well as SET, AT, and HAT processes, will be investigated under this award. It is believed that these methods, when fully developed, will not only deepen our understanding of electron-transfer chemistry, but they will also substantially broaden the tools that are available for the synthesis and late-stage modification of complex molecules and drugs.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.

在化学系化学合成计划的支持下，弗拉基米尔Gevorgyan教授和他在德克萨斯大学达拉斯分校的研究生和本科生正在开发温和，高效和选择性的合成有机分子的反应方法。特别是，Gevorgyan小组正在开发有机化学方法，以将具有丰富碳氢（C-H）键的现成原料化学品转化为其他更有价值的化学品，这些化学品含有在药物和材料中更常见的新键（碳-氧（C-O）、碳-氮（C-N）、碳-卤素（C-X）、碳-碳（C-C）、碳-硼（C-B）等）。为了实现这些转化，Gevorgyan教授的团队正在开发一种反应方法，这种方法不需要昂贵的、可能有毒的和/或爆炸性的试剂。除了提供新的和有效的途径来构建复杂的分子和重要的材料，拟议的工作的更广泛的影响包括外联活动，旨在招募本科生，包括代表性不足的少数民族学生，进入研究，他们的潜力和职业机会将得到提高。Gevorgyan团队正在开发新的温和方法，用于产生以碳原子和杂原子为中心的自由基，并释放它们的反应性。正在开发的方法依赖于新的供体-受体（DA）复合物，能够使用单电子转移（SET）还原亲电中间体。他们的工作正在使用可见光引发进行，导致产生经历原子转移（AT）或氢原子转移（HAT）以产生转置自由基的前体自由基。这些新的自由基可以参与许多不同的合成转化，包括C（sp3）−H键官能化反应。该奖项将研究有利于DA复合物有效形成的因素，以及SET，AT和HAT过程。相信这些方法一旦得到充分发展，不仅将加深我们对电子转移化学的理解，而且还将大大拓宽复杂分子和药物的合成和后期修饰的工具。该奖项反映了NSF的法定使命，并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，被认为值得支持。