Vibrational spectroscopy reveals the initial steps of biological hydrogen evolution

Sagie Katz, Jens Noth, Marius Horch, Hannah Shafaat, Thomas Happe, Peter Hildebrandt & Ingo Zebger
[FeFe] hydrogenases are biocatalytic model systems for the exploitation and investigation of catalytic hydrogen evolution. Here, we used vibrational spectroscopic techniques to characterize, in detail, redox transformations of the [FeFe] and [4Fe4S] sub-sites of the catalytic centre (H-cluster) in a monomeric [FeFe] hydrogenase. Through the application of low-temperature resonance Raman spectroscopy, we discovered a novel metastable intermediate that is characterized by an oxidized [(FeFeII)-Fe-I] centre and a reduced [4Fe4S](1+) cluster. Based on this unusual configuration,...
This data repository is not currently reporting usage information. For information on how your repository can submit usage information, please see our documentation.