Engineering and Evolving Dirhodium Artificial Metalloenzymes for Carbene Transfer Reactions

David Matthew Upp
This dissertation describes the engineering and evolution of dirhodium artificial metalloenzymes (ArMs) for selective carbene transfer catalysis. The ArM hybrid catalyst is formed by covalent attachment of a dirhodium tetracarboxylate cofactor a prolyl oligopeptidase scaffold, which is shown to control the environment around the metal center to enable selectivity. The process of improving this scaffold-based control through multiple carbene transfer reactions has improved our understanding of this system and ArMs more broadly. Chapter 1 begins...
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