New Approaches to Catalyst Screening and Development

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This project will continue work on the development of catalyst screening methods that employ enzymes as the analytical sensors. This approach has been labeled In Situ Enzymatic Screening (ISES). While chromatographic screening methods are established, these are normally run as serial, time point assays, requiring aliquot removal and work-up, prior to analysis. The ISES method offers the possibility to obtain parallel, real time estimates of relative reaction rates and, in ideal cases, sense and magnitude of enantio-induction, without the need to install a chromophore or mass tag in the substrate. A key goal of the next cycle of this project is to enhance the throughput of the ISES screening, such that larger matrices of potential catalytic combinations may be screened. Also important will be to further develop the most interesting catalysts uncovered in the last cycle, including carbohydrate-based chiral salen ligands, and new combinations of late transition metal halides for formal halocarbocyclization processes. In addition, further expansion of the scope of chemistry that is amenable to screening via ISES will be investigated.With this award, the Organic and Macromolecular Chemistry Program is supporting the research of Professor David B. Berkowitz in the Department of Chemistry at the University of Nebraska. Professor Berkowitz's research efforts include the development of useful new catalysts for the stereo-controlled opening of small ring compounds, and for carbon-halogen and carbon-carbon bond formation. Successful development of the methodology will have an impact on synthesis in both the academic and industrial communities, the latter particularly in the combinatorial catalysis and pharmaceutical process areas.