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CO synthesized from the central one-carbon pool as source for the iron carbonyl in O 2 -tolerant [NiFe]-hydrogenase
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| Zeitschriftentitel: | Proceedings of the National Academy of Sciences |
|---|---|
| Personen und Körperschaften: | , , , , , |
| In: | Proceedings of the National Academy of Sciences, 113, 2016, 51, S. 14722-14726 |
| Format: | E-Article |
| Sprache: | Englisch |
| veröffentlicht: |
Proceedings of the National Academy of Sciences
|
| Schlagwörter: |
| author_facet |
Bürstel, Ingmar Siebert, Elisabeth Frielingsdorf, Stefan Zebger, Ingo Friedrich, Bärbel Lenz, Oliver Bürstel, Ingmar Siebert, Elisabeth Frielingsdorf, Stefan Zebger, Ingo Friedrich, Bärbel Lenz, Oliver |
|---|---|
| author |
Bürstel, Ingmar Siebert, Elisabeth Frielingsdorf, Stefan Zebger, Ingo Friedrich, Bärbel Lenz, Oliver |
| spellingShingle |
Bürstel, Ingmar Siebert, Elisabeth Frielingsdorf, Stefan Zebger, Ingo Friedrich, Bärbel Lenz, Oliver Proceedings of the National Academy of Sciences CO synthesized from the central one-carbon pool as source for the iron carbonyl in O 2 -tolerant [NiFe]-hydrogenase Multidisciplinary |
| author_sort |
bürstel, ingmar |
| spelling |
Bürstel, Ingmar Siebert, Elisabeth Frielingsdorf, Stefan Zebger, Ingo Friedrich, Bärbel Lenz, Oliver 0027-8424 1091-6490 Proceedings of the National Academy of Sciences Multidisciplinary http://dx.doi.org/10.1073/pnas.1614656113 <jats:title>Significance</jats:title> <jats: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 <jats:sub>2</jats: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) <jats:sub>2</jats: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. </jats:p> CO synthesized from the central one-carbon pool as source for the iron carbonyl in O <sub>2</sub> -tolerant [NiFe]-hydrogenase Proceedings of the National Academy of Sciences |
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| title |
CO synthesized from the central one-carbon pool as source for the iron carbonyl in O 2 -tolerant [NiFe]-hydrogenase |
| title_unstemmed |
CO synthesized from the central one-carbon pool as source for the iron carbonyl in O 2 -tolerant [NiFe]-hydrogenase |
| title_full |
CO synthesized from the central one-carbon pool as source for the iron carbonyl in O 2 -tolerant [NiFe]-hydrogenase |
| title_fullStr |
CO synthesized from the central one-carbon pool as source for the iron carbonyl in O 2 -tolerant [NiFe]-hydrogenase |
| title_full_unstemmed |
CO synthesized from the central one-carbon pool as source for the iron carbonyl in O 2 -tolerant [NiFe]-hydrogenase |
| title_short |
CO synthesized from the central one-carbon pool as source for the iron carbonyl in O 2 -tolerant [NiFe]-hydrogenase |
| title_sort |
co synthesized from the central one-carbon pool as source for the iron carbonyl in o
<sub>2</sub>
-tolerant [nife]-hydrogenase |
| topic |
Multidisciplinary |
| url |
http://dx.doi.org/10.1073/pnas.1614656113 |
| publishDate |
2016 |
| physical |
14722-14726 |
| description |
<jats:title>Significance</jats:title>
<jats: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
<jats:sub>2</jats: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)
<jats:sub>2</jats: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.
</jats:p> |
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| author | Bürstel, Ingmar, Siebert, Elisabeth, Frielingsdorf, Stefan, Zebger, Ingo, Friedrich, Bärbel, Lenz, Oliver |
| author_facet | Bürstel, Ingmar, Siebert, Elisabeth, Frielingsdorf, Stefan, Zebger, Ingo, Friedrich, Bärbel, Lenz, Oliver, Bürstel, Ingmar, Siebert, Elisabeth, Frielingsdorf, Stefan, Zebger, Ingo, Friedrich, Bärbel, Lenz, Oliver |
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| container_title | Proceedings of the National Academy of Sciences |
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| description | <jats:title>Significance</jats:title> <jats: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 <jats:sub>2</jats: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) <jats:sub>2</jats: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. </jats:p> |
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| imprint_str_mv | Proceedings of the National Academy of Sciences, 2016 |
| institution | DE-D275, DE-Bn3, DE-Brt1, DE-Zwi2, DE-D161, DE-Zi4, DE-Gla1, DE-15, DE-Pl11, DE-Rs1, DE-14, DE-105, DE-Ch1, DE-L229 |
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| spelling | Bürstel, Ingmar Siebert, Elisabeth Frielingsdorf, Stefan Zebger, Ingo Friedrich, Bärbel Lenz, Oliver 0027-8424 1091-6490 Proceedings of the National Academy of Sciences Multidisciplinary http://dx.doi.org/10.1073/pnas.1614656113 <jats:title>Significance</jats:title> <jats: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 <jats:sub>2</jats: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) <jats:sub>2</jats: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. </jats:p> CO synthesized from the central one-carbon pool as source for the iron carbonyl in O <sub>2</sub> -tolerant [NiFe]-hydrogenase Proceedings of the National Academy of Sciences |
| spellingShingle | Bürstel, Ingmar, Siebert, Elisabeth, Frielingsdorf, Stefan, Zebger, Ingo, Friedrich, Bärbel, Lenz, Oliver, Proceedings of the National Academy of Sciences, CO synthesized from the central one-carbon pool as source for the iron carbonyl in O 2 -tolerant [NiFe]-hydrogenase, Multidisciplinary |
| title | CO synthesized from the central one-carbon pool as source for the iron carbonyl in O 2 -tolerant [NiFe]-hydrogenase |
| title_full | CO synthesized from the central one-carbon pool as source for the iron carbonyl in O 2 -tolerant [NiFe]-hydrogenase |
| title_fullStr | CO synthesized from the central one-carbon pool as source for the iron carbonyl in O 2 -tolerant [NiFe]-hydrogenase |
| title_full_unstemmed | CO synthesized from the central one-carbon pool as source for the iron carbonyl in O 2 -tolerant [NiFe]-hydrogenase |
| title_short | CO synthesized from the central one-carbon pool as source for the iron carbonyl in O 2 -tolerant [NiFe]-hydrogenase |
| title_sort | co synthesized from the central one-carbon pool as source for the iron carbonyl in o <sub>2</sub> -tolerant [nife]-hydrogenase |
| title_unstemmed | CO synthesized from the central one-carbon pool as source for the iron carbonyl in O 2 -tolerant [NiFe]-hydrogenase |
| topic | Multidisciplinary |
| url | http://dx.doi.org/10.1073/pnas.1614656113 |