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

Christian Lorent, Sagie Katz, Jifu Duan, Catharina Julia Kulka, Giorgio Caserta, Christian Teutloff, Shanika Yadav, Ulf Peter Apfel, Martin Winkler, Thomas Happe, Marius Horch, Ingo Zebger

Research output: Contribution to journalArticlepeer-review


[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.

Original languageEnglish
Pages (from-to)5493-5497
Number of pages5
JournalJournal of the American Chemical Society
Issue number12
Early online date3 Mar 2020
Publication statusPublished - 25 Mar 2020

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