Department Seminar – Theo Agapie, California Institute of Technology, Thursday, December 15, 2022, 1:30-2:30
Dec 15, 2022
1:30PM to 2:30PM
Date/Time
Date(s) - 15/12/2022
1:30 pm - 2:30 pm
Title: Synthetic Cluster Models of Protein Active Sites
Date: Thursday, December 15, 2022
Room: ABB 165 (in-person only)
Host: David Emslie
Abstract: Complex inorganic active sites perform challenging catalytic transformations in biological systems, such as water oxidation by Photosystem II and nitrogen reduction in Nitrogenase. The effect of cluster structure on the physical and chemical properties of these active sites is not well understood. We have developed methodologies for the rational synthesis of tetra- and pentanuclear homo- and hetero-metallic cluster models of protein active sites, which allow for systematic structure-property studies. Clusters displaying the cubane motif found in the Oxygen Evolving Complex (OEC) have been prepared, and the redox inactive metal was found to impact redox chemistry. Tetranuclear clusters that structurally model the dangler motif of the OEC have also been synthesized, with open coordination sites for water coordination. Distal redox changes have been demonstrated to have a substantial effect on the reactivity and binding of ligands relevant to small molecule conversions. Upon incorporation of second coordination sphere hydrogen bonding interactions, water oxidation catalysis was observed. Spectroscopic studies of models with structures or redox states relevant to the protein active site provide benchmarking for the biological system. Implications for function and spectroscopy will be discussed.
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