Inhibition of the [NiFe] hydrogenase from Desulfovibrio vulgaris Miyazaki F by carbon monoxide: an FTIR and EPR spectroscopic study

Biochimica Et Biophysica Acta
Maria-Eirini PandeliaWolfgang Lubitz

Abstract

X-ray crystallographic studies [Ogata et al., J. Am. Chem. Soc. 124 (2002) 11628-11635] have shown that carbon monoxide binds to the nickel ion at the active site of the [NiFe] hydrogenase from Desulfovibriovulgaris Miyazaki F and inhibits its catalytic function. In the present work spectroscopic aspects of the CO inhibition for this bacterial organism are reported for the first time and enable a direct comparison with the existing crystallographic data. The binding affinity of each specific redox state for CO is probed by FTIR spectro-electrochemistry. It is shown that only the physiological state Ni-SI(a) reacts with CO. The CO-inhibited product state is EPR-silent (Ni2+) and exists in two forms, Ni-SCO and Ni-SCO(red). At very negative potentials, the exogenous CO is electrochemically detached from the active site and the active Ni-R states are obtained. At temperatures below 100 K, photodissociation of the extrinsic CO from the Ni-SCO state results in Ni-SI(a) that is identified to be the only light-induced state. In the dark, rebinding of CO takes place; the recombination rate constants are of biexponential character and the activation barrier is determined to be approximately 9 kJ mol(-1). In addition, formation of a para...Continue Reading

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Citations

Aug 9, 2011·Applied Microbiology and Biotechnology·Ya ZhaoSerge R Guiot
Feb 7, 2012·Inorganic Chemistry·David SchilterMatthias Stein
Jul 30, 2010·Journal of Biological Inorganic Chemistry : JBIC : a Publication of the Society of Biological Inorganic Chemistry·Cristina Gutiérrez-SánchezInês A C Pereira
Apr 8, 2015·Chemistry : a European Journal·Claire Wombwell, Erwin Reisner
Oct 1, 2015·Inorganic Chemistry·Geoffrey M ChambersWolfgang Lubitz
Jul 28, 2015·The Journal of Physical Chemistry. B·Julia LöwensteinRobert Bittl
Dec 17, 2014·The Journal of Chemical Physics·Olaseni Sode, Gregory A Voth
Nov 20, 2012·Biochemical and Biophysical Research Communications·Hisao OsukaShun Hirota
Feb 13, 2013·Biochimica Et Biophysica Acta·Hannah S ShafaatWolfgang Lubitz
Nov 2, 2016·Journal of Biochemistry·Hideaki OgataYoshiki Higuchi
Sep 21, 2016·Journal of the American Chemical Society·Matteo SensiLuca Bertini
Oct 9, 2015·Chemical Communications : Chem Comm·Carlo U PerottoMartin Schröder
Jul 21, 2017·Dalton Transactions : an International Journal of Inorganic Chemistry·Li-Cheng SongXu-Yong Wang
Mar 14, 2018·Dalton Transactions : an International Journal of Inorganic Chemistry·Hulin TaiShun Hirota
Sep 6, 2018·Physical Chemistry Chemical Physics : PCCP·Siyao QiuChenghua Sun
Mar 20, 2010·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Maria-Eirini PandeliaWolfgang Lubitz
Aug 19, 2017·Australian Journal of Chemistry·David SchilterThomas B Rauchfuss
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Aug 23, 2011·Inorganic Chemistry·Takahiro MatsumotoSeiji Ogo
Jul 9, 2014·Journal of the American Chemical Society·Suzannah V HexterFraser A Armstrong
Oct 4, 2017·Journal of Inorganic Biochemistry·Nikolay A ZorinAnatoly A Tsygankov

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