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.
