PMID: 11929218Apr 4, 2002Paper

Hydrogen-bond-mediated tuning of the redox potential of the non-heme Fe site of superoxide dismutase

Journal of the American Chemical Society
Emine YikilmazA F Miller

Abstract

The highly homologous proteins of Fe-containing superoxide dismutase (FeSOD) and MnSOD from Escherichia coli nonetheless exert very different redox tuning on the active site metal ion [Vance; Miller J. Am. Chem. Soc. 1998, 120, 461-467; Biochemistry 2001, 40, 13079-13087]. This was proposed to stem from different hydrogen bonding between the protein and the metal ion's coordinated solvent molecule, and the tight coupling between the protonation state of coordinated solvent and the oxidation state of the metal ion. We now present density functional theory (DFT) calculations on Fe2+ and Fe3+ bound to models of both FeSOD and MnSOD. The calculations support a very important role for the conserved second sphere Gln in MnSOD in specifically destabilizing coordinated H2O relative to coordinated OH-, and thus disfavouring the oxidized state of the metal ion. To test these results we have mutated this Gln to Glu, which is isosteric and isoelectronic to Gln but functions as an H-bond acceptor instead of an H-bond donor and thus should increase the stability of Fe2+-bound H2O. In accordance with the calculations, Q69E-FeSOD displays a significantly higher reduction potential than wild-type FeSOD. Thus we have demonstrated that hydrogen b...Continue Reading

Citations

Apr 6, 2004·Current Opinion in Chemical Biology·Anne-Frances Miller
Nov 15, 2011·Journal of the American Chemical Society·Yuewei ShengJoan Selverstone Valentine
Aug 8, 2008·Chemical Communications : Chem Comm·Luciano CuestaJonathan L Sessler
Nov 15, 2011·FEBS Letters·Anne-Frances Miller
May 11, 2010·Biochimica Et Biophysica Acta·Masaki OsawaB Yukihiro Hiraoka
Nov 26, 2009·Biochimica Et Biophysica Acta·Anne-Frances MillerSurekha Vathyam
Jan 22, 2005·Protein Science : a Publication of the Protein Society·Inés G MuñozGuillermo Montoya
Aug 25, 2015·Biochimica Et Biophysica Acta·Parisa Hosseinzadeh, Yi Lu
Jul 12, 2017·Protein Science : a Publication of the Protein Society·Takahide YamaguchiTakamitsu Kohzuma
Jun 28, 2006·Journal of Computational Chemistry·Lubomír RulísekUlf Ryde
Jul 11, 2006·Journal of Biological Inorganic Chemistry : JBIC : a Publication of the Society of Biological Inorganic Chemistry·Louis Noodleman, Wen-Ge Han
Sep 7, 2019·Molecular Informatics·Maria J R Yunta, Roque Carlos Dietrich
Nov 16, 2007·The Journal of Biological Chemistry·Nicholas P TuckerRay Dixon
Jul 7, 2005·Journal of the American Chemical Society·Christian R GoldsmithT Daniel P Stack
Apr 2, 2014·Chemical Reviews·Yuewei ShengJoan Selverstone Valentine
Apr 14, 2005·Journal of the American Chemical Society·Adam T FiedlerThomas C Brunold
Dec 12, 2002·Journal of the American Chemical Society·James MaliekalAnne-Frances Miller
Jun 15, 2006·The Journal of Physical Chemistry. B·Lubomír Rulísek, Ulf Ryde
Jul 14, 2007·Journal of the American Chemical Society·Emine YikilmazAnne-Frances Miller
Apr 4, 2002·Journal of the American Chemical Society·Juan XieThomas C Brunold

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