A supramolecular approach to combining enzymatic and transition metal catalysis

Author:  ["Z. Jane Wang","Kristen N. Clary","Robert G. Bergman","Kenneth N. Raymond","F. Dean Toste"]

Publication:  Nature Chemistry

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Tags:     Chemistry

Abstract

The ability of supramolecular host–guest complexes to catalyse organic reactions collaboratively with an enzyme is an important goal in the research and discovery of synthetic enzyme mimics. Herein we present a variety of catalytic tandem reactions that employ esterases, lipases or alcohol dehydrogenases and gold(I) or ruthenium(II) complexes encapsulated in a Ga4L6 tetrahedral supramolecular cluster. The host–guest complexes are tolerated well by the enzymes and, in the case of the gold(I) host–guest complex, show improved reactivity relative to the free cationic guest. We propose that supramolecular encapsulation of organometallic complexes prevents their diffusion into the bulk solution, where they can bind amino-acid residues on the proteins and potentially compromise their activity. Our observations underline the advantages of the supramolecular approach and suggest that encapsulation of reactive complexes may provide a general strategy for carrying out classic organic reactions in the presence of biocatalysts. Combinations of enzymatic and chemo-catalysis can result in powerful synthetic transformations. Here, encapsulation of Au(I) or Ru(II) within a supramolecular assembly prevents diffusion of the organometallic complexes into solution where they can compromise the activity of an enzyme. This strategy has been applied to tandem reactions employing supramolecular host–guest complexes and enzymes in the catalysis of organic transformations.

Cite this article

Wang, Z., Clary, K., Bergman, R. et al. A supramolecular approach to combining enzymatic and transition metal catalysis. Nature Chem 5, 100–103 (2013). https://doi.org/10.1038/nchem.1531

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