Mechanism of Enantioselective Catalysis with Cu(II)

Enantioselective catalysis forms a highly competitive field in synthetic organic chemistry. This is because stereo- (or enantio-)selective catalysis is a very convenient way to synthesize chiral molecules. Such molecules generally exhibit biological or pharmacological activity. Therefore, the research on the development of new catalysts is a field of intense scientific work. Surprisingly, only rarely investigations target the mechanisms behind these catalytic processes. This is particularly because standard approaches are not appropriate to handle the complex interplay of several factors participating in a catalytic cycle. In our project, we introduce a combination of modern, advanced state-of-the-art experimental and theoretical methodologies to provide a detailed insight into the intrinsic characteristics of catalysis: to unravel the subtle influence of metal atoms, ligands, dynamics of the coordination sphere, solvent participation, and counterions within the course of catalytic reactions. All experiments will be performed under "real" synthetic conditions, however at a smaller scale to allow performing these reactions in reactors which fit into spectrometers. The reactions will be followed by magnetic- resonance methods like EPR, FT-ENDOR, and HYSCORE, optical spectroscopy and NMR. Theoretical calculations based at the density-functional level of theory will be utilized to obtain further insights at the molecular level. It is our aim to contribute to the development of innovative, efficient ligands and the optimization of experimental conditions.

Enantioselective catalysis forms a highly competitive field in synthetic organic chemistry. This is because stereo- (or enantio-)selective catalysis is a very convenient way to synthesize chiral molecules. Such molecules generally exhibit biological or pharmacological activity. Therefore, the research on the development of new catalysts is a field of intense scientific work. Surprisingly, only rarely investigations target the mechanisms behind these catalytic processes. This is particularly because standard approaches are not appropriate to handle the complex interplay of several factors participating in a catalytic cycle. In our project, we introduce a combination of modern, advanced state-of-the-art experimental and theoretical methodologies to provide a detailed insight into the intrinsic characteristics of catalysis: to unravel the subtle influence of metal atoms, ligands, dynamics of the coordination sphere, solvent participation, and counterions within the course of catalytic reactions. All experiments will be performed under "real" synthetic conditions, however at a smaller scale to allow performing these reactions in reactors which fit into spectrometers. The reactions will be followed by magnetic-resonance methods like EPR, FT-ENDOR, and HYSCORE, optical spectroscopy and NMR. Theoretical calculations based at the density-functional level of theory will be utilized to obtain further insights at the molecular level. It is our aim to contribute to the development of innovative, efficient ligands and the optimization of experimental conditions.