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  Dioxygen Sensitivity of [Fe]‐Hydrogenase in the Presence of Reducing Substrates

Huang, G., Wagner, T., Ermler, U., Bill, E., Ataka, K., & Shima, S. (2018). Dioxygen Sensitivity of [Fe]‐Hydrogenase in the Presence of Reducing Substrates. Angewandte Chemie International Edition in English, 57(18), 4917-4920. doi:10.1002/anie.201712293.

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 Urheber:
Huang, Gangfeng1, Autor
Wagner, Tristan1, Autor
Ermler, Ulrich2, Autor                 
Bill, Eckhard3, Autor
Ataka, Kenichi4, Autor
Shima, Seiko1, Autor
Affiliations:
1Max-Planck-Institut für terrestrische Mikrobiologie, Karl-von-Frisch-Straße 10, 35043 Marburg, Germany, ou_persistent22              
2Department of Molecular Membrane Biology, Max Planck Institute of Biophysics, Max Planck Society, ou_2068290              
3Max-Planck-Institut für Chemische Energiekonversion, 45470 Mühlheim, Germany, ou_persistent22              
4Department of Physics, Freie Universität Berlin, 14195 Berlin, Germany, ou_persistent22              

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Schlagwörter: [Fe]-hydrogenase;·enzyme catalysis ·H2; hydrogenation; O2 sensitivity
 Zusammenfassung: Mono‐iron hydrogenase ([Fe]‐hydrogenase) reversibly catalyzes the transfer of a hydride ion from H2 to methenyltetrahydromethanopterin (methenyl‐H4MPT+) to form methylene‐H4MPT. Its iron guanylylpyridinol (FeGP) cofactor plays a key role in H2 activation. Evidence is presented for O2 sensitivity of [Fe]‐hydrogenase under turnover conditions in the presence of reducing substrates, methylene‐H4MPT or methenyl‐H4MPT+/H2. Only then, H2O2 is generated, which decomposes the FeGP cofactor; as demonstrated by spectroscopic analyses and the crystal structure of the deactivated enzyme. O2 reduction to H2O2 requires a reductant, which can be a catalytic intermediate transiently formed during the [Fe]‐hydrogenase reaction. The most probable candidate is an iron hydride species; its presence has already been predicted by theoretical studies of the catalytic reaction. The findings support predictions because the same type of reduction reaction is described for ruthenium hydride complexes that hydrogenate polar compounds

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Sprache(n): eng - English
 Datum: 2017-11-302018-02-202018-03-222018-04-23
 Publikationsstatus: Erschienen
 Seiten: 4
 Ort, Verlag, Ausgabe: -
 Inhaltsverzeichnis: -
 Art der Begutachtung: Expertenbegutachtung
 Identifikatoren: DOI: 10.1002/anie.201712293
 Art des Abschluß: -

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Titel: Angewandte Chemie International Edition in English
  Kurztitel : Angew. Chem. Int. Ed. Engl.
Genre der Quelle: Zeitschrift
 Urheber:
Affiliations:
Ort, Verlag, Ausgabe: Weinheim : Wiley-VCH
Seiten: - Band / Heft: 57 (18) Artikelnummer: - Start- / Endseite: 4917 - 4920 Identifikator: ISSN: 0570-0833
CoNE: https://pure.mpg.de/cone/journals/resource/0570-0833