Catalytic C-H Amination with Late Metal Nitrenes and Amides

在这个由化学部化学催化项目资助的项目中，乔治城大学的Timothy H. Warren教授将开发催化碳氢（C-H）胺化反应，作为制备新的碳氮（C-N）键的一种手段，而不需要对反应位点进行预功能化。直接影响C-H到C-N转化的能力，而不需要分离、纯化和转化相应的前体，这为降低成本、能耗和环境影响提供了诱人的前景。在先前结果的基础上，这种方法将铜和镍硝基和酰胺配合物的化学和电子结构与其催化反应性联系起来。这项工作特别研究了从有机叠氮化物衍生的铜和硝基镍配合物，反应的胺和底物范围，以及新的催化剂结构，以进一步提高催化反应的效率和范围。该项目的更广泛影响包括国内和国际合作，这将扩大学生对科学在更大的科学界中进行的方式的看法。沃伦教授积极指导高中生、本科生（特别是通过nsf赞助的REU项目）和研究生。这项工作将扩大可用于含有C-N键的化合物的化学合成方法的曲目。这些研究的结果可能对合成化学和材料化学的各种应用产生许多重要的长期影响，特别是在医药或制药产品方面。

In this project funded by the Chemical Catalysis Program of the Chemistry Division, Professor Timothy H. Warren of Georgetown University will develop catalytic carbon-hydrogen (C-H) amination reactions as a means of preparing new carbon-nitrogen (C-N) bonds without the need to pre-functionalize the reactive sites. The ability to directly affect the C-H to C-N transformation without the need to isolate, purify, and transform corresponding precursors offers the appealing prospect of reduced cost, energy consumption and environmental impact. Building on previous results, this approach connects the chemical and electronic structures of copper and nickel nitrene and amide complexes to their catalytic reactivity. The work specifically examines copper and nickel nitrene complexes derived from organoazides, the amine and substrate scope of the reactions, and new catalysts architectures to further enhance the efficiency and scope of the catalytic reactions. The broader impacts of this project include national and international collaborations that will expand the student's perspective on the way science is conducted within the larger scientific community. Professor Warren is active in mentoring high school students, undergraduates (especially through the NSF-sponsored REU program) and graduate students.This work will expand the repertoire of methods that can be used in the chemical synthesis of compounds containing C-N bonds. The results of these studies could have many important long term impacts on a variety of applications in synthetic and materials chemistry, particularly in medicinal or pharmaceutical products.