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

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Author(s)

  • 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

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Publication details

JournalJournal of the American Chemical Society
DateAccepted/In press - 3 Mar 2020
DateE-pub ahead of print - 3 Mar 2020
DatePublished (current) - 25 Mar 2020
Issue number12
Volume142
Number of pages5
Pages (from-to)5493-5497
Early online date3/03/20
Original languageEnglish

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.

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© 2020 American Chemical Society. This is an author-produced version of the published paper. Uploaded in accordance with the publisher’s self-archiving policy. Further copying may not be permitted; contact the publisher for details.

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