Bio-inspired Electron-delivering System for Reductive Activation of Dioxygen at Metal Centres Towards Artificial Flavoenzymes

Overview

Journal Nat Commun

Specialty Biology

Date 2015 Oct 1

PMID 26419885

Citations 3

Authors

Yoann Roux

Remy Ricoux

Frederic Avenier

Jean-Pierre Mahy

Affiliations

Soon will be listed here.

Abstract

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

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