Development of Positional Selective C-H Activation Reactions

有了这个奖项，化学系的化学催化计划正在资助斯克里普斯研究所的Jin-Quan Yu教授开发新的反应，将有机分子中的碳氢键转化为各种更复杂的化学结构。这些转化是合成用于药物、精细化学品和农用化学品的分子的重要工具，控制碳-氢键官能化的化学反应一直是化学界面临的长期挑战。 该研究项目的其他更广泛的影响包括学生和博士后研究人员培训，小学生外展计划，以及邀请高中生在夏天在实验室进行研究。余教授正在开发方法，对钯配合物的弱配位促进的遥远和几何上不可接近的碳-氢键进行位点选择性官能化，继续进行一系列的研究，这些研究已经导致了沿着这些路线的一些第一批这样的成功。具体而言，研究正集中在使用基于腈的模板的间碳氢（C-H）活化过程上。首先，新的腈模板正在开发和广泛优化以前不成功的基板。第二，正在开发新的配体和条件，以实现具有挑战性的转化，如间碳-氢羰基化。第三，深入了解如何腈模板指导远程碳氢活化寻求表征的大元环化中间体，以及寻求通过计算工作，以确定过渡态结构。 如果成功的话，这些研究中开发的方法可以在工业和工业的化学方法/合成实验室中得到广泛的应用。

With this award, the Chemical Catalysis Program of the Division of Chemistry is funding Professor Jin-Quan Yu of The Scripps Research Institute to develop new reactions that convert carbon-hydrogen bonds in organic molecules into a wide range of more complex chemical structures. These transformations are important tools for the synthesis of molecules that are used in pharmaceuticals, fine chemicals, and agrochemicals, and controlling the chemistry of carbon-hydrogen bond functionalization has been a long-standing challenge for the chemistry community. Additional broader impacts of the research project include student and postdoctoral researcher training, an outreach program to elementary students, and inviting high-school students to perform research in the laboratory over the summer.Professor Yu is developing methods to perform the site-selective functionalization of remote and geometrically inaccessible carbon-hydrogen bonds promoted by weak coordination of palladium complexes, continuing a linge of research which has led to some of the first such successes along these lines. Specifically, research is being focused on meta-carbon-hydrogen (C-H) activation processes using nitrile-based templates. First, new nitrile templates are being developed and extensively optimized for previously unsuccessful substrates. Second, new ligands and conditions are being developed to enable challenging transformations such as meta-carbon-hydrogen carbonylation. Third, an in-depth understanding of how the nitrile template directs remote carbon-hydrogen activation is sought by characterizing the large-membered cyclometalation intermediates as well as seeking to identify the transition state structures through computational efforts. If successful, the methods being developed in these studies could find broad application in chemical methods/synthesis laboratories in both academe and industry.