Bio-inspired electron-delivering system for reductive activation of dioxygen at metal centres towards artificial flavoenzymes
Yoann Roux, Rémy Ricoux, Frédéric Avenier & Jean-Pierre Mahy
Nature Communications 6, Article number : 8509
doi:10.1038/ncomms9509
Received
Accepted
Published
http://www.nature.com/ncomms/2015/150930/ncomms9509/full/ncomms9509.html
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.
Nature Communications 6, Article number : 8509
doi:10.1038/ncomms9509
Received
Accepted
Published
http://www.nature.com/ncomms/2015/150930/ncomms9509/full/ncomms9509.html
Abstract
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