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An S-Oxygenated [NiFe] Complex Modelling Sulfenate Intermediates of an O2-Tolerant Hydrogenase
Citation key ANIE:ANIE201611069
Author Lindenmaier, Nils J. and Wahlefeld, Stefan and Bill, Eckhard and Szilvási, Tibor and Eberle, Christopher and Yao, Shenglai and Hildebrandt, Peter and Horch, Marius and Zebger, Ingo and Driess, Matthias
Pages 2208–2211
Year 2017
ISSN 1521-3773
DOI 10.1002/anie.201611069
Journal Angewandte Chemie International Edition
Volume 56
Number 8
Abstract To understand the molecular details of O2-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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