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Synthetic cluster models of the biological oxygen evolving complex: Insights regarding function and spectroscopy

Agapie, Theodor (2020) Synthetic cluster models of the biological oxygen evolving complex: Insights regarding function and spectroscopy. In: 259th ACS National Meeting & Exposition, 22-26 March 2020, Philadelphia, PA. https://resolver.caltech.edu/CaltechAUTHORS:20200219-081913734

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Abstract

Complex inorg. active sites perform challenging catalytic transformations in biol. systems, such as water oxidn. by Photosystem II and nitrogen redn. in Nitrogenase. The effect of cluster structure on the phys. and chem. 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 the Oxygen Evolving Complex in Photosystem II, which allow for systematic structure-property studies. Clusters displaying the cubane motif found in the OEC have been prepd., and the redox inactive metal was found to impact redox chem. Tetranuclear clusters that structurally model the dangler motif 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 of aquo, hydroxide, and oxo ligands relevant to water oxidn. Upon incorporation of second coordination sphere hydrogen bonding interactions, water oxidn. catalysis was obsd. Spectroscopic studies of models with structures or redox states relevant to the OEC provide benchmarking for the biol. system. Implications for the function and spectroscopy of the OEC will be discussed.


Item Type:Conference or Workshop Item (Paper)
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ORCID:
AuthorORCID
Agapie, Theodor0000-0002-9692-7614
Additional Information:© 2020 American Chemical Society.
Record Number:CaltechAUTHORS:20200219-081913734
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20200219-081913734
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:101361
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:19 Feb 2020 17:48
Last Modified:19 Feb 2020 17:48

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