Bio-inspired electron-delivering system for reductive activation of dioxygen at metal centres towards artificial flavoenzymes

Flavin mononucleotide Electron acceptor Biocatalysis
DOI: 10.1038/ncomms9509 Publication Date: 2015-09-30T10:33:43Z
ABSTRACT
Abstract Development of artificial systems, capable delivering electrons to metal-based catalysts for the reductive activation dioxygen, has been proven very difficult decades, constituting a major scientific lock elaboration environmentally friendly oxidation processes. Here we demonstrate that incorporation flavin mononucleotide (FMN) in water-soluble polymer, bearing locally hydrophobic microenvironment, allows efficient reduction FMN by NADH. This supramolecular entity is then catalysing fast single-electron manganese(III) porphyrin splitting electron pair issued from fully reminiscent activity natural reductases such as cytochrome P450 with kinetic parameters, which are three orders magnitude faster compared other systems. Finally, show proof concept reduced manganese activates dioxygen and catalyses organic substrates water.
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