CO synthesized from the central one-carbon pool as source for the iron carbonyl in O2-tolerant [NiFe]-hydrogenase
Identifieur interne : 000762 ( Ncbi/Checkpoint ); précédent : 000761; suivant : 000763CO synthesized from the central one-carbon pool as source for the iron carbonyl in O2-tolerant [NiFe]-hydrogenase
Auteurs : Ingmar Bürstel [Allemagne] ; Elisabeth Siebert [Allemagne] ; Stefan Frielingsdorf [Allemagne] ; Ingo Zebger [Allemagne] ; B Rbel Friedrich [Allemagne] ; Oliver Lenz [Allemagne]Source :
- Proceedings of the National Academy of Sciences of the United States of America [ 0027-8424 ] ; 2016.
Abstract
Activation of dihydrogen is by far not a trivial catalytic reaction. Microbes have evolved sophisticated hydrogenases with complex transition metal centers to get access to H2. A recurring feature of these centers is the presence of iron atoms equipped with carbon monoxide ligands. In case of [NiFe]-hydrogenases, which contain a NiFe(CN)2CO catalytic center, biosynthesis of the toxic CO ligand remained elusive. We show that [NiFe]-hydrogenases that are catalytically active in the presence of dioxygen use a dedicated maturase for CO ligand synthesis under aerobic conditions. CO is derived from the most oxidized intermediate of the central one-carbon metabolism, formyl-tetrahydrofolate. This discovery contributes a so far unknown reaction to the one-carbon metabolism and opens perspectives for chemical and of bioinspired catalysis.
Url:
DOI: 10.1073/pnas.1614656113
PubMed: 27930319
PubMed Central: 5187695
Affiliations:
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<country xml:lang="fr">Allemagne</country>
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-tolerant [NiFe]-hydrogenase</title>
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<series><title level="j">Proceedings of the National Academy of Sciences of the United States of America</title>
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<front><div type="abstract" xml:lang="en"><title>Significance</title>
<p>Activation of dihydrogen is by far not a trivial catalytic reaction. Microbes have evolved sophisticated hydrogenases with complex transition metal centers to get access to H<sub>2</sub>
. A recurring feature of these centers is the presence of iron atoms equipped with carbon monoxide ligands. In case of [NiFe]-hydrogenases, which contain a NiFe(CN)<sub>2</sub>
CO catalytic center, biosynthesis of the toxic CO ligand remained elusive. We show that [NiFe]-hydrogenases that are catalytically active in the presence of dioxygen use a dedicated maturase for CO ligand synthesis under aerobic conditions. CO is derived from the most oxidized intermediate of the central one-carbon metabolism, formyl-tetrahydrofolate. This discovery contributes a so far unknown reaction to the one-carbon metabolism and opens perspectives for chemical and of bioinspired catalysis.</p>
</div>
</front>
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<name sortKey="Burstel, Ingmar" sort="Burstel, Ingmar" uniqKey="Burstel I" first="Ingmar" last="Bürstel">Ingmar Bürstel</name>
<name sortKey="Friedrich, B Rbel" sort="Friedrich, B Rbel" uniqKey="Friedrich B" first="B Rbel" last="Friedrich">B Rbel Friedrich</name>
<name sortKey="Frielingsdorf, Stefan" sort="Frielingsdorf, Stefan" uniqKey="Frielingsdorf S" first="Stefan" last="Frielingsdorf">Stefan Frielingsdorf</name>
<name sortKey="Frielingsdorf, Stefan" sort="Frielingsdorf, Stefan" uniqKey="Frielingsdorf S" first="Stefan" last="Frielingsdorf">Stefan Frielingsdorf</name>
<name sortKey="Lenz, Oliver" sort="Lenz, Oliver" uniqKey="Lenz O" first="Oliver" last="Lenz">Oliver Lenz</name>
<name sortKey="Lenz, Oliver" sort="Lenz, Oliver" uniqKey="Lenz O" first="Oliver" last="Lenz">Oliver Lenz</name>
<name sortKey="Siebert, Elisabeth" sort="Siebert, Elisabeth" uniqKey="Siebert E" first="Elisabeth" last="Siebert">Elisabeth Siebert</name>
<name sortKey="Zebger, Ingo" sort="Zebger, Ingo" uniqKey="Zebger I" first="Ingo" last="Zebger">Ingo Zebger</name>
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