EXAFS and NRVS reveal a conformational distortion of the FeMo-cofactor in the MoFe nitrogenase propargyl alcohol complex.

Journal of Inorganic Biochemistry
Simon J GeorgeLance C Seefeldt

Abstract

We have used EXAFS and NRVS spectroscopies to examine the structural changes in the FeMo-cofactor active site of the α-70(Ala) variant of Azotobacter vinelandii nitrogenase on binding and reduction of propargyl alcohol (PA). The Mo K-edge near-edge and EXAFS spectra are very similar in the presence and absence of PA, suggesting PA does not bind at Mo. By contrast, Fe EXAFS spectra show a clear and reproducible change in the long Fe-Fe interaction at ~3.7 Å on PA binding with the apparent appearance of a new Fe-Fe interaction at 3.99 Å. An analogous change in the long Mo-Fe 5.1 Å interaction is not seen. The NRVS spectra exclude the possibility of large-scale structural change of the FeMo-cofactor involving breaking the μ(2) Fe-S-Fe bonds of the Fe(6)S(9)X core. The simplest chemically consistent structural change is that the bound form of PA is coordinated at Fe atoms (Fe6 or Fe7) adjacent to the Mo terminus, with a concomitant movement of the Fe away from the central atom X and along the Fe-X bond by about 0.35 Å. This study comprises the first experimental evidence of the conformational changes of the FeMo-cofactor active site on binding a substrate or product.

References

Feb 11, 2004·Biochemistry·Lance C SeefeldtDennis R Dean
Jun 1, 2005·Biochemistry·Brett M BarneyLance C Seefeldt

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Citations

Feb 22, 2014·Journal of Biological Inorganic Chemistry : JBIC : a Publication of the Society of Biological Inorganic Chemistry·Oliver Einsle
Sep 18, 2013·Proceedings of the National Academy of Sciences of the United States of America·Jonathan Rittle, Jonas C Peters
Dec 9, 2014·Biochimica Et Biophysica Acta·Joanna Kowalska, Serena DeBeer
May 14, 2016·Journal of the American Chemical Society·Ilija Čorić, Patrick L Holland
Sep 4, 2014·Journal of the American Chemical Society·Jonathan RittleJonas C Peters
Apr 22, 2015·Dalton Transactions : an International Journal of Inorganic Chemistry·Ian Dance
Sep 30, 2015·Nature·Ilija ČorićPatrick L Holland
Dec 6, 2019·Chembiochem : a European Journal of Chemical Biology·Ian Dance
Oct 17, 2013·Chemical Communications : Chem Comm·Ian Dance

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