1. SEP_Shedding Light on Proton and Electron Dynamics in [FeFe] Hydrogenases
- Author
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Lorent, Christian, Katz, Sagie, Duan, Jifu, Kulka, Catharina Julia, Caserta, Giorgio, Teutloff, Christian, Yadav, Shanika, Apfel, Ulf-Peter, Winkler, Martin, Happe, Thomas, Horch, Marius, and Zebger, Ingo
- Subjects
[FeFe] Hydrogenase ,500 Naturwissenschaften und Mathematik::530 Physik::530 Physik ,cryogenic infrared spectroscopy ,electron paramagnetic resonance spectroscopy ,reversible dihydrogen evolution ,catalysts - Abstract
[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.
- Published
- 2020
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