Final - Development of Regioselective Alkene Dicarbofunctionalization Reactions

项目摘要/摘要 在母公司的奖励下，我们正在开发未活化的烯烃的催化二碳功能化，这是一种强大的 一步生成两个碳-碳键的方法。机械性调查一直是研究的主要内容 以便我们更好地理解和改进这些催化反应。我们在我们的 机理研究是通过原位~(19)F-核磁共振波谱实时分析反应过程。这 策略使我们能够识别反应中间体，并同时测量 想要的产品、区域下滑的产品和不想要的副产品。我们充分利用了这一关键的机制 了解催化循环的微妙之处并确定适当的反应参数以改进 并扩大父母拨款中提出的反应范围。然而，我们在机械学方面的进展 分析受到长期核磁共振保留的限制和全天候访问 我们核磁共振设施中的专用核磁共振谱仪。我们预计收购所要求的牛津60号 MHZ X-脉冲核磁共振波谱仪，能够对我们感兴趣的多个核(1H、19F、11B和31P)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，使 迅速取得重大进展，有助于填补烯烃领域的重大知识空白 二碳官能化对达到母公司拨款目标的反应。

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.