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An S-Oxygenated [NiFe] Complex Modelling Sulfenate Intermediates of an O-2-Tolerant Hydrogenase
Zitatschlüssel ISI:000397323300045
Autor Lindenmaier, Nils J. and Wahlefeld, Stefan and Bill, Eckhard and Szilvasi, Tibor and Eberle, Christopher and Yao, Shenglai and Hildebrandt, Peter and Horch, Marius and Zebger, Ingo and Driess, Matthias
Seiten 2208-2211
Jahr 2017
ISSN 1433-7851
DOI 10.1002/ange.201611069
Adresse POSTFACH 101161, 69451 WEINHEIM, GERMANY
Journal ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Jahrgang 56
Nummer 8
Monat FEB 13
Verlag WILEY-V C H VERLAG GMBH
Zusammenfassung To understand the molecular details of O-2-tolerant hydrogen cycling by a soluble NAD(+)-reducing [NiFe] hydrogenase, we herein present the first bioinspired heterobimetallic S-oxygenated [NiFe] complex as a structural and vibrational spectroscopic model for the oxygen-inhibited [NiFe] active site. This compound and its non-S-oxygenated congener were fully characterized, and their electronic structures were elucidated in a combined experimental and theoretical study with emphasis on the bridging sulfenato moiety. Based on the vibrational spectroscopic properties of these complexes, we also propose novel strategies for exploring S-oxygenated intermediates in hydrogenases and similar enzymes.
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