Final - Development of Regioselective Alkene Dicarbofunctionalization Reactions

项目总结/摘要 在母公司的奖励下，我们正在开发未活化烯烃的催化双碳官能化，这是一种强大的 在一个步骤中产生两个碳-碳键的方法。机械研究一直是研究的主要内容 让我们更好地理解和改进这些催化反应。我们实施的一项关键战略是， 机理研究是通过原位19 F NMR光谱实时分析反应进程。这 这一策略使我们能够识别反应中间体，并同时测量生成的速率。 期望的产物、区域滑移产物和不期望的副产物。我们利用这个关键的机械 知识，了解催化循环的微妙之处，并确定合适的反应参数，以提高 并扩大父母补助金中提出的反应范围。然而，我们在机械方面的进展 由于长期核磁共振保留和24/7访问的限制，分析受到严重阻碍。 在我们的核磁共振设施专用核磁共振光谱仪。我们预计，收购所要求的牛津60 MHz X-Pulse NMR光谱仪，能够在100 MHz下对我们感兴趣的多个核（1H，19 F，11B和31 P）进行采样。 可变的温度，将极大地缓解我们的局限性，增加我们的研究能力， 迅速取得重大进展，有助于填补烯烃领域的重大知识空白 二碳功能化反应对满足父母补助金的目标。

Project Summary/Abstract Under the parent award, we are developing catalytic dicarbofunctionalization of unactivated alkenes, a powerful method to create two carbon-carbon bonds in one step. Mechanistic investigations have been a research staple for us to better understand and improve these catalytic reactions. One of the key strategies we implement in our mechanistic studies is the analysis of reaction progress in real-time by in-situ 19F NMR spectroscopy. This strategy allows us to identify reaction intermediates, and measure simultaneously the rates of formation of desired products, regio-slipped products and undesired side products. We capitalize on this critical mechanistic knowledge to understand the subtleties of a catalytic cycle and identify suitable reaction parameters to improve and expand the scope of the reactions proposed in the parent grant. However, our progress in mechanistic analysis has been seriously hampered by limitations on long-term NMR reservations and 24/7 access to a dedicated NMR spectrometer in our NMR facility. We anticipate that the acquisition of the requested Oxford 60 MHz X-Pulse NMR spectrometer, capable of sampling multiple nuclei of interest to us (1H, 19F, 11B and 31P) at variable temperature, will tremendously ease on our limitations, increase our research capacity to make significant progress rapidly, and help fill in a significant knowledge gap in the field of alkene dicarbofunctionalization reactions toward meeting the goals of the parent grant.