NEW SYNTHESIS OF BIOCHEMICAL WITH HOMOGENEOUS CATALYSTS

我们的最终目标是设计和开发多功能多功能 催化剂系统，使我们能够进行多步合成， 以高度有组织的方式一锅烩。 作为一项基本 为了实现这一具有挑战性的目标，我们将发起和促进 “均相合成生物化学品新方法”的研究 催化剂”。 该项目包括四个子项目。 (i)阐发 通过立体化学方法研究了酰胺羰基化的机理 方法，在其中我们将解决一个历史之谜，即，水 在高浓度的H2O存在下， 通过设计双环中间体， 严格的空间要求， 区分可能提出的机制。 (ii)螯合- 在羰基化反应中的定向区域和立体控制，其中我们 将首次系统地引入螯合控制， 并将其应用于催化不对称 合成. (iii)分子内酰胺羰基化反应的应用 氮杂环的合成，我们将在其中开发 合成生物活性物质的有效新方法 含氮杂环，尤其是生物碱的中间体。 (iv)CoRh（CO）7反应机理的高压FT-IR研究 这种独特的混合金属簇的催化行为 将研究关于水文- 酰胺羰基化方法。

Our ultimate goal is to design and develop multi-functional multi- catalyst systems which enable us to carry out multi-step synthesis in one-pot in a highly organized manner. As a fundamental approach to this challenging goal, we will initiate and promote the research on the "new synthesis of biochemicals with homogeneous catalysts". This project includes four subprojects. (i) Elucidation of the mechanism of amidocarbonylation by stereochemical approach, in which we will solve 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 so that we can unambiguously distinguish the possible mechanisms proposed. (ii) Chelation- directed regio- and stereocontrol in carbonylations, in which we will systematically introduce chelation control, for the first time, to carbonylations and apply it to the catalytic asymmetric synthesis. (iii) Applications of intramolecular amidocarbonylation' to the synthesis of nitrogen heterocycles, in which we will develop efficient new methods for the synthesis of biologically active nitrogen heterocyles, especially the intermediates for alkaloids. (iv) High pressure FT-IR study on the mechanism of CoRh(CO)7 catalysis in which the behavior of this unique mixed-metal cluster will be studied regarding the hydroformylation- amidocarbonylation process.