Following [FeFe] Hydrogenase Active Site Intermediates by Time-Resolved Mid-IR Spectroscopy

Mohammad Mirmohades, Agnieszka Adamska-Venkatesh, Constanze Sommer, Edward Reijerse, Reiner Lomoth, Wolfgang Lubitz, Leif Hammarström

Research output: Contribution to journalArticle

8 Citations (Scopus)

Abstract

Time-resolved nanosecond mid-infrared spectroscopy is for the first time employed to study the [FeFe] hydrogenase from Chlamydomonas reinhardtii and to investigate relevant intermediates of the enzyme active site. An actinic 355 nm, 10 ns laser flash triggered photodissociation of a carbonyl group from the CO-inhibited state Hox-CO to form the state Hox, which is an intermediate of the catalytic proton reduction cycle. Time-resolved infrared spectroscopy allowed us to directly follow the subsequent rebinding of the carbonyl, re-forming Hox-CO, and determine the reaction half-life to be t1/2 ≈ 13 ± 5 ms at room temperature. This gives direct information on the dynamics of CO inhibition of the enzyme.

Original languageEnglish
Pages (from-to)3290-3293
Number of pages4
JournalJournal of Physical Chemistry Letters
Volume7
Issue number16
DOIs
Publication statusPublished - Aug 18 2016

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Hydrogenase
Carbon Monoxide
enzymes
Infrared spectroscopy
Enzymes
infrared spectroscopy
Photodissociation
Enzyme inhibition
half life
photodissociation
spectroscopy
flash
Protons
cycles
protons
Lasers
room temperature
lasers
Temperature

ASJC Scopus subject areas

  • Materials Science(all)

Cite this

Following [FeFe] Hydrogenase Active Site Intermediates by Time-Resolved Mid-IR Spectroscopy. / Mirmohades, Mohammad; Adamska-Venkatesh, Agnieszka; Sommer, Constanze; Reijerse, Edward; Lomoth, Reiner; Lubitz, Wolfgang; Hammarström, Leif.

In: Journal of Physical Chemistry Letters, Vol. 7, No. 16, 18.08.2016, p. 3290-3293.

Research output: Contribution to journalArticle

Mirmohades M, Adamska-Venkatesh A, Sommer C, Reijerse E, Lomoth R, Lubitz W et al. Following [FeFe] Hydrogenase Active Site Intermediates by Time-Resolved Mid-IR Spectroscopy. Journal of Physical Chemistry Letters. 2016 Aug 18;7(16):3290-3293. https://doi.org/10.1021/acs.jpclett.6b01316
Mirmohades, Mohammad ; Adamska-Venkatesh, Agnieszka ; Sommer, Constanze ; Reijerse, Edward ; Lomoth, Reiner ; Lubitz, Wolfgang ; Hammarström, Leif. / Following [FeFe] Hydrogenase Active Site Intermediates by Time-Resolved Mid-IR Spectroscopy. In: Journal of Physical Chemistry Letters. 2016 ; Vol. 7, No. 16. pp. 3290-3293.
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