Synthetic and Mechanistic Studies on the Homogenous Catalysis of Transition Metal Complexes (Chemistry)

过渡金属均相催化的研究 将由有机和高分子化学 程序. 开发新的基于 催化体系具有提供更经济， 无污染的合成方法 工业和农业材料。 最终目标是设计开发多功能 多催化剂系统，其将允许多步合成， 以高度有组织的方式一锅。 这个项目包括 三个分项目：㈠混合金属的机理研究 以CoRh（CO）7机理为中心的催化剂体系 包括高压FT-IR催化行为的研究 关于这个独特的混合金属复合体的 加氢甲酰化-酰胺基-羰基化方法;（ii） 酰胺羰基化反应机理的研究 立体化学的方法，将解决一个历史性的 神秘，即，水选择性地裂解酰基钴键 高压氢气的存在，通过设计双环 具有严格空间要求的中间体， 明确区分可能的机制 （三）螯合导向的区域和立体控制 在羰基化反应中， 螯合控制，第一次，羰基化， 将其应用于催化不对称合成。

This research on transition metals for homogeneous catalysis will be supported by the Organic and Macromolecular Chemistry Program. The development of new synthetic tools based on catalytic systems has the potential to provide more economic, pollution-free methods for the synthesis of the complex materials for industry and agriculture. The ultimate goal is to design and develop multi-functional multicatalyst systems which will permit multi-step synthesis in one-pot in a highly organized manner. This project includes three sub-projects: (i) mechanistic study of mixed metal catalyst systems focusing on the mechanism of CoRh(CO)7 catalysis including high pressure FT-IR study on the behavior of this unique mixed-metal complex regarding the hydroformylation-amido-carbonylation process; (ii) elucidation of the mechanism of amidocarbonylation by stereochemical approach which will resolve a historical mystery, i.e., water cleaves acylcobalt bond selectively in the presence of high pressure hydrogen, by designing bicyclic intermediates bearing strict steric requirements that can unambiguously distinguish among the possible mechanisms proposed; (iii) chelation-directed regio- and stereocontrol in carbonylations, which will systematically introduce chelation control, for the first time, to carbonylations and apply it to the catalytic asymmetric synthesis.