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De novo biosynthesis of a nonnatural cobalt porphyrin cofactor in <i>E. coli</i> and incorporation into hemoproteins

Lydia J. Perkins, Brian R. Weaver, Andrew R. Buller, Judith N. Burstyn

2021Proceedings of the National Academy of Sciences27 citationsDOIOpen Access PDF

Abstract

(FePPIX). Five cobalt-substituted proteins were successfully expressed with this new-to-nature cobalt porphyrin cofactor: myoglobin H64V V68A, dye decolorizing peroxidase, aldoxime dehydratase, cytochrome P450 119, and catalase. We show conclusively that these proteins incorporate CoPPIX, with the CoPPIX making up at least 95% of the total porphyrin content. In cases in which the native metal ligand is a sulfur or nitrogen, spectroscopic parameters are consistent with retention of native metal ligands. This method is an improvement on previous approaches with respect to both yield and ease-of-implementation. Significantly, this method overcomes a long-standing challenge to incorporate nonnatural cofactors through de novo biosynthesis. By utilizing a ubiquitous laboratory strain, this process will facilitate spectroscopic studies and the development of enzymes for CoPPIX-mediated biocatalysis.

Topics & Concepts

CofactorPorphyrinHemeHemeproteinChemistryCobaltMetalloproteinBiocatalysisDehydrataseBiosynthesisBiochemistryMyoglobinStereochemistryEscherichia coliLigand (biochemistry)EnzymeCombinatorial chemistryOrganic chemistryReaction mechanismCatalysisGeneReceptorMetal-Catalyzed Oxygenation MechanismsPorphyrin Metabolism and DisordersPorphyrin and Phthalocyanine Chemistry
De novo biosynthesis of a nonnatural cobalt porphyrin cofactor in <i>E. coli</i> and incorporation into hemoproteins | Litcius