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

doi:10.1021/jacs.9b13075

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

Chemistry

Research output: Contribution to journal › Article › peer-review

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.

Original language	English
Pages (from-to)	5493-5497
Number of pages	5
Journal	Journal of the American Chemical Society
Volume	142
Issue number	12
Early online date	3 Mar 2020
DOIs	https://doi.org/10.1021/jacs.9b13075
Publication status	Published - 25 Mar 2020

Bibliographical note

© 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.

Access to Document

10.1021/jacs.9b13075

Lorent_et_al_accepted
© 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.
Accepted author manuscript, 439 KB

Cite this

@article{1d29ccc0b3904f998658554be155e729,

title = "Shedding Light on Proton and Electron Dynamics in [FeFe] Hydrogenases",

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.",

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

note = "{\textcopyright} 2020 American Chemical Society. This is an author-produced version of the published paper. Uploaded in accordance with the publisher{\textquoteright}s self-archiving policy. Further copying may not be permitted; contact the publisher for details.",

year = "2020",

month = mar,

day = "25",

doi = "10.1021/jacs.9b13075",

language = "English",

volume = "142",

pages = "5493--5497",

journal = "Journal of the American Chemical Society",

issn = "0002-7863",

publisher = "American Chemical Society",

number = "12",

}

TY - JOUR

T1 - Shedding Light on Proton and Electron Dynamics in [FeFe] Hydrogenases

AU - Lorent, Christian

AU - Katz, Sagie

AU - Duan, Jifu

AU - Kulka, Catharina Julia

AU - Caserta, Giorgio

AU - Teutloff, Christian

AU - Yadav, Shanika

AU - Apfel, Ulf Peter

AU - Winkler, Martin

AU - Happe, Thomas

AU - Horch, Marius

AU - Zebger, Ingo

N1 - © 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.

PY - 2020/3/25

Y1 - 2020/3/25

N2 - [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.

AB - [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.

UR - http://www.scopus.com/inward/record.url?scp=85082387164&partnerID=8YFLogxK

U2 - 10.1021/jacs.9b13075

DO - 10.1021/jacs.9b13075

M3 - Article

C2 - 32125830

AN - SCOPUS:85082387164

SN - 0002-7863

VL - 142

SP - 5493

EP - 5497

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

IS - 12

ER -

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

Abstract

Bibliographical note

Access to Document

Other files and links

Cite this