Mechanistic features and structure of the nitrogenase alpha-Gln195 MoFe protein

Biochemistry
Morten SørlieBrian J Hales

Abstract

EPR signals observed under CO and C(2)H(2) during nitrogenase turnover were investigated for the alpha-Gln(195) MoFe protein, an altered form for which the alpha-His(195) residue has been substituted by glutamine. Under CO, samples show S = 1/2 hi- and lo-CO EPR signals identical to those recognized for the wild-type protein, whereas the S = 3/2 signals generated under high CO/high flux conditions differ. Previous work has revealed that the EPR spectrum generated under C(2)H(2) exhibits a signal (S(EPR1)) originating from the FeMo-cofactor having two or more bound C(2)H(2) adducts and a second signal (S(EPR2)) arising from a radical species [Sørlie, M., Christiansen, J., Dean, D. R., and Hales, B. J. (1999) J. Am. Chem. Soc. 121, 9457-9458]. Pressure-dependent studies show that the intensity of these signals has a sigmoidal dependency at low pressures and maximized at 0.1 atm C(2)H(2) with a subsequent decrease in steady-state intensity at higher pressures. Analogous signals are not recognized for the wild-type MoFe protein. Analysis of the principal g-factors of S(EPR2) suggests that it either represents an unusual metal cluster or is a carboxylate centered radical possibly originating from homocitrate. Both S(EPR1) and S(EPR2...Continue Reading

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Citations

May 12, 2005·Journal of Biological Inorganic Chemistry : JBIC : a Publication of the Society of Biological Inorganic Chemistry·Zofia MaskosBrian J Hales
Jan 23, 2003·Journal of Inorganic Biochemistry·Zofia Maskos, Brian J Hales
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Mar 10, 2009·Accounts of Chemical Research·Brian M HoffmanLance C Seefeldt
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Jun 6, 2009·Annual Review of Biochemistry·Lance C SeefeldtDennis R Dean
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Dec 6, 2019·Chembiochem : a European Journal of Chemical Biology·Ian Dance
Oct 17, 2013·Chemical Communications : Chem Comm·Ian Dance
May 2, 2020·Acta Crystallographica. Section D, Structural Biology·Wan Ting JinZhao Hui Zhou
Mar 17, 2020·Chemical Reviews·Lance C SeefeldtBrian M Hoffman
Apr 3, 2020·Chemical Reviews·Casey Van StappenSerena DeBeer
Oct 18, 2020·Journal of Inorganic Biochemistry·Derek F HarrisLance C Seefeldt
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