New Approaches to Catalyst Screening and Development

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TECHNICAL SUMMARY:With this award the National Science Foundation is funding studies at the University of Nebraska, under the direction of Professor Stephen G. DiMagno (substitute PI for Professor David Berkowitz), to develop new enzyme-based methods for catalyst screening. This approach involves the use of enzymatic reporting enzymes operating in tandem with the organic/organometallic catalysts being screened, with the former in an aqueous reporting layer, and the latter in an organic solvent layer within the same vessel. This arrangement permits for the assessment of key variables including relative reaction rate and enantioselectivity, in real time, and is thus termed "In Situ Enzymatic Screening" (ISES). Particular focus here is on the identification of new screening enzymes/conditions that will permit the experimentalist to examine new leaving groups and new transformations and to move from ambient to elevated temperatures. Transformations being targeted include those of particular interest to bioorganic and medicinal chemists, such as catalytic routes to enantio-enriched, quaternary, alpha-vinyl amino acids as potential mechanism-based enzyme inhibitors.NON-TECHNICAL SUMMARY:This research project is inherently interdisciplinary, at the interface between organic chemistry and biology, as Nature's catalysts are exploited to assist with the development of useful human-made catalysts for chemical synthesis. Scientists working on the project will gain hands-on experience with both frontline asymmetric catalyst development and with modern preparative enzymology. The research is expected to have broader scientific impact on the areas of organic synthesis, green chemistry, biocatalysis, and process chemistry. The PI will continue to provide cross-disciplinary training to postdocs, graduate, and undergraduate students, and the group will continue to reach out to high school students through Chemistry Day.