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-Jespersen在无机、生物无机和有机金属化学项目的支持下，开发了能够激活C-H键并在随后的反应中形成C-C键的催化剂。通过氧化加成活化C-H和通过还原消除形成C-C键是该体系实现C-H到C-C转化的基本步骤。本项目利用PCP螯合Ir配合物作为C-H活化的首选平台，并将设计新的Ru配合物来完成相关的C-H活化和C-C成键反应。本研究探讨了还原消除形成新的碳-碳键的机理细节，以建立促进碳-碳键形成的指导方针。由于碳氢键在有机化合物中无处不在，通过激活和操纵这些相对惰性的键，它们为碳-碳框架结构提供了丰富的来源。该项目的广泛影响包括对从高中到研究生的各级参与者的教育效益，包括计算技能，实验复杂的合成技术，以及结合无机和有机机械探针建立专业知识的机会。

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.