Artificial organometallic proteins afford the opportunity to harness the diverse reactivity of abiotic transition metals within the complex and selective, yet modular and easily accessible, environment of a protein. Despite this potential, examples of expedient methods for the preparation of well-defined, protein-ligated late transition metal catalysts are rare in the literature. Moreover, the reported methods used to characterize these constructs are limited, impeding the study and improvement of catalytic activity. In further development of this desirable class of catalysts, new methods for the preparation and characterization of well-defined artificial organometallic proteins derived from late transition metal precursors and natural metalloprotein scaffolds are disclosed. Using these methods, selective metallation has been achieved at a single site within the protein scaffold, resulting in the formation of a discrete catalytic environment. Furthermore, the novel use of a series of solution-state characterization techniques has allowed the detailed characterization of the nature of the organometallic complex contained within the protein matrix. This expansion of characterization methods to define artificial organometallic proteins in the reaction state has enabled our subsequent study of their participation in fundamental organometallic reactions that compose catalytic cycles. The understanding that we gain from these reactivity studies will facilitate the future development of catalysts with higher activity and selectivity.

Artificial organometallic proteins: Characterization and fundamental reactivity

248th National Meeting (2014)

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