Mechanism Study Of Rh(I) Carbene Trapping Active Intermediate Three-compound Reaction

Multi-component reactions (MCRs) is one typical represent of green chemistry because of the advantages of highly efficient synthetic strategies, atom economy, easy operation and so on. Recently, MCRs has received more and more attention. However, the computational mechanism study of MCRs is much rare. Computational mechanism study has a great meaning to experiments because it could help cut cost of experiments and widen substrate scope of reactions. In past several decades, thanks to the development of computer, computational chemistry-has been playing an important role in various aspects of chemical study. Density Functional Theory (DFT) became very popular in aspect of mechanism study for its great performance in predicting structures and energies of molecules.In this thesis, DFT is applied to study the first Rh(I)-catalyzed three-compound reaction reported by our group. The most reasonable reaction path is decided by calculating structures and energies of intermediates and transition state.The construction of molecule models is based on experimental results and empirical mechanism. The thesis focuses on four problems:1. The specific structure of intermediate trapped by the third component.2. The pattern the third compound interacts with metal catalyst and the way the selectivity of stereochemistry arise.3. The specific pattem of hydrogen transfer.4. The selectivity of metal catalysts.