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Shedding Light on Proton and Electron Dynamics in [FeFe] Hydrogenases
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| Journal | Journal of the American Chemical Society |
|---|---|
| Date | Accepted/In press - 3 Mar 2020 |
| Date | E-pub ahead of print - 3 Mar 2020 |
| Date | Published (current) - 25 Mar 2020 |
| Issue number | 12 |
| Volume | 142 |
| Number of pages | 5 |
| Pages (from-to) | 5493-5497 |
| Early online date | 3/03/20 |
| Original language | English |
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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