The development of a viable chemical catalyst for water oxidation are currently being pursued to store energy in the form of the chemical bonds within H2 and O2. Extensive work in synthetic chemistry has shown that mononuclear and μ-oxo-bridged dinuclear Ru complexes are capable of electrocatalytically splitting H2O through the formation of high valent Ru centers. However, the efficacy of synthetic Ru water-oxidation catalysts (WOCs) is often limited by obstacles such as complex aggregation and ligand displacement. Nature overcomes these challenges by sequestering reactive complexes within protein hosts where a more controlled environment confers uniform, efficient, and reproducible reactivity. This presentation will discuss strategies employed for the design of a Ru artificial metalloprotein (ArM) that may serve as an efficient WOC. Using biotin-Streptavidin (Sav) technology, a RuIII complex has been immobilized within the Sav protein host. Site-direct mutation provides Sav variants with endogenous ligands from the peptide sidechain that bind the artificial RuIII complexes to aid in fixing its location within the protein. Spectroscopic evidence for RuIII-S bond formation will be discussed and an outline of the experimental path to catalysis with the Ru-ArM is detailed.

Design and synthesis of a ruthenium artificial metalloprotein using biotin-streptavidin technology

ACS Spring 2022

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