Oxygen activation by a mixed-valent, diiron(II/III) cluster in the glycol cleavage reaction catalyzed by myo-inositol oxygenase

Biochemistry
Gang XingJ Martin Bollinger

Abstract

myo-Inositol oxygenase (MIOX) catalyzes the ring-cleaving, four-electron oxidation of its cyclohexan-(1,2,3,4,5,6-hexa)-ol substrate (myo-inositol, MI) to d-glucuronate (DG). The preceding paper [Xing, G., Hoffart, L. M., Diao, Y., Prabhu, K. S., Arner, R. J., Reddy, C. C., Krebs, C., and Bollinger, J. M., Jr. (2006) Biochemistry 45, 5393-5401] demonstrates by Mössbauer and electron paramagnetic resonance (EPR) spectroscopies that MIOX can contain a non-heme dinuclear iron cluster, which, in its mixed-valent (II/III) and fully oxidized (III/III) states, is perturbed by binding of MI in a manner consistent with direct coordination. In the study presented here, the redox form of the enzyme that activates O(2) has been identified. l-Cysteine, which was previously reported to accelerate turnover, reduces the fully oxidized enzyme to the mixed-valent form, and O(2), the cosubstrate, oxidizes the fully reduced form to the mixed-valent form with a stoichiometry of one per O(2). Both observations implicate the mixed-valent, diiron(II/III) form of the enzyme as the active state. Stopped-flow absorption and freeze-quench EPR data from the reaction of the substrate complex of mixed-valent MIOX [MIOX(II/III).MI] with limiting O(2) in the p...Continue Reading

References

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Citations

Feb 7, 2012·Biochemistry·Laura M K DassamaJ Martin Bollinger
Apr 13, 2010·Inorganic Chemistry·Anusree MukherjeeLawrence Que
May 9, 2012·Journal of the American Chemical Society·Fern R McSorleyDavid L Zechel
May 16, 2013·Journal of the American Chemical Society·Wei-chen ChangHung-wen Liu
Jun 12, 2009·Nature·Robert M CicchilloWilliam W Metcalf
Apr 21, 2009·Chemical Communications : Chem Comm·Sachin A Joshi, Neelima D Kulkarni
Nov 8, 2013·Proceedings of the National Academy of Sciences of the United States of America·Bigna WörsdörferMaria-Eirini Pandelia
Mar 28, 2008·The Journal of Biological Chemistry·Ann-Gerd ThorsellB Martin Hallberg
Aug 2, 2011·Yakugaku zasshi : Journal of the Pharmaceutical Society of Japan·Hajime Hirao, Keiji Morokuma
Oct 3, 2006·Proceedings of the National Academy of Sciences of the United States of America·Peter M BrownEdward N Baker
Dec 26, 2013·Coordination Chemistry Reviews·Carsten KrebsJ Martin Bollinger
Mar 22, 2007·Current Opinion in Chemical Biology·J Martin Bollinger, Carsten Krebs
Oct 19, 2010·Current Opinion in Structural Biology·Wilfred A van der DonkJ Martin Bollinger
Jan 29, 2009·Dalton Transactions : an International Journal of Inorganic Chemistry·J Martin BollingerCarsten Krebs
May 21, 2016·Journal of the American Chemical Society·Anna J KomorJohn D Lipscomb
Jul 3, 2016·Journal of Biological Inorganic Chemistry : JBIC : a Publication of the Society of Biological Inorganic Chemistry·Edward I Solomon, Kiyoung Park
Nov 17, 2016·Proceedings of the National Academy of Sciences of the United States of America·Jennifer Bridwell-RabbCatherine L Drennan
Oct 21, 2009·Journal of the American Chemical Society·John T WhitteckWilfred A van der Donk
Jun 7, 2008·Journal of Chemical Information and Modeling·Joannis ApostolakisJohann Gasteiger
Sep 13, 2014·Journal of the American Chemical Society·Kallol RayWonwoo Nam

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