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Shedding Light on Proton and Electron Dynamics in [FeFe] Hydrogenases

: Lorent, C.; Katz, S.; Duan, J.; Kulka, C.J.; Caserta, G.; Teutloff, C.; Yadav, S.; Apfel, U.-P.; Winkler, M.; Happe, T.; Horch, M.; Zebger, I.


Journal of the American Chemical Society 142 (2020), Nr.12, S.5493-5497
ISSN: 0002-7863
ISSN: 1520-5126
Fraunhofer UMSICHT Oberhausen ()

[FeFe] hydrogenases are highly efficient catalysts for reversible dihydrogen evolution. H2 turnover involves different catalytic intermediates including a recently characterized hydride state of the active site (H-cluster). Applying cryogenic infrared and electron paramagnetic resonance spectroscopy to an [FeFe] model hydrogenase from Chlamydomonas reinhardtii (CrHydA1), we have discovered two new hydride intermediates and spectroscopic evidence for a bridging CO ligand in two reduced H-cluster states. Our study provides novel insights into these key intermediates, their relevance for the catalytic cycle of [FeFe] hydrogenase, and novel strategies for exploring these aspects in detail.