Development of catalysts for the transformation of C-H to C-C bonds; experimental and computational studies of relevant fundamental reaction steps including C-C bond elimination

罗格斯大学的Alan Goldman教授和他的同事Karsten Krogh-Jesperen在无机、生物无机和金属有机化学计划的支持下开发了催化剂，这些催化剂将允许C-H键的活化，并在随后的反应中导致C-C键的形成。通过氧化加成活化C-H和通过还原消除形成C-C键的步骤是在该体系中实现C-H到C-C转化的基本步骤。该项目利用PCP钳形连接的Ir络合物作为C-H活化的首选平台，并将设计新的Ru络合物来完成相关的C-H活化和C-C键形成反应。本研究对还原消除形成新的C-C键的机理细节进行了探讨，以建立促进碳-碳键形成的指导方针。由于C-H键普遍存在于有机化合物中，它们通过激活和操纵这些相对惰性的键为碳-碳骨架的构建提供了丰富的来源。该项目的更广泛影响包括对所有级别的参与者的教育好处，从高中到研究生，包括计算技能、实验上复杂的合成技术，以及通过结合无机和有机机械探头积累专业知识的机会。

Professor Alan Goldman of Rutgers University and his colleague Karsten Krogh-Jespersen are supported by the Inorganic, Bioinorganic and Organometallic Chemistry program to develop catalysts that will allow the activation of C-H bonds and lead to the formation of C-C bonds in subsequent reactions. The separate steps of C-H activation via oxidative addition and C-C bond formation via reductive elimination are the essential steps set forth for realizing C-H to C-C transformations in this system. This project utilizes PCP pincer ligated Ir complexes as the preferred platform for C-H activation, and new Ru complexes will be designed to accomplish related C-H activation and C-C bond forming reactions. The mechanistic details of reductive elimination to form new C-C bonds are being probed in this study in order to establish guidelines for promoting carbon-carbon bond formation.Since C-H bonds are ubiquitous in organic compounds they provide a rich source for carbon-carbon framework constructions by activation and manipulation of these relatively inert bonds. The broader impacts of this project include educational benefits for all levels of participants, from high school through graduate students, that include computational skills, experimentally sophisticated synthetic techniques, and opportunities to build expertise with a combination of inorganic and organic mechanistic probes.