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Direct Detection of the Terminal Hydride Intermediate in [FeFe] Hydrogenase by NMR Spectroscopy

Author:
Rumpel, Sigrun, Sommer, Constanze, Reijerse, Edward, Farès, Christophe, Lubitz, Wolfgang
Source:
Journal of the American Chemical Society 2018 v.140 no.11 pp. 3863-3866
ISSN:
1520-5126
Subject:
Chlamydomonas reinhardtii, ambient temperature, enzymes, hydrides, hydrogen, nuclear magnetic resonance spectroscopy
Abstract:
Hydride state intermediates are known to occur in various hydrogen conversion enzymes, including the highly efficient [FeFe] hydrogenases. The intermediate state involving a terminal iron-bound hydride has been recognized as crucial for the catalytic mechanism, but its occurrence has up to now eluded unequivocal proof under (near) physiological conditions. Here we show that the terminal hydride in the [FeFe] hydrogenase from Chlamydomonas reinhardtii can be directly detected using solution ¹H NMR spectroscopy at room temperature, opening new avenues for detailed in situ investigations under catalytic conditions.
Agid:
6033120