A coupled dinuclear iron cluster that is perturbed by substrate binding in myo-inositol oxygenase

Biochemistry
Gang XingJ Martin Bollinger

Abstract

myo-Inositol oxygenase (MIOX) uses iron as its cofactor and dioxygen as its cosubstrate to effect the unique, ring-cleaving, four-electron oxidation of its cyclohexan-(1,2,3,4,5,6-hexa)-ol substrate to d-glucuronate. The nature of the iron cofactor and its interaction with the substrate, myo-inositol (MI), have been probed by electron paramagnetic resonance (EPR) and Mössbauer spectroscopies. The data demonstrate the formation of an antiferromagnetically coupled, high-spin diiron(III/III) cluster upon treatment of solutions of Fe(II) and MIOX with excess O(2) or H(2)O(2) and the formation of an antiferromagnetically coupled, valence-localized, high-spin diiron(II/III) cluster upon treatment with either limiting O(2) or excess O(2) in the presence of a mild reductant (e.g., ascorbate). Marked changes to the spectra of both redox forms upon addition of MI and analogy to changes induced by binding of phosphate to the diiron(II/III) cluster of the protein phosphatase, uteroferrin, suggest that MI coordinates directly to the diiron cluster, most likely in a bridging mode. The addition of MIOX to the growing family of non-heme diiron oxygenases expands the catalytic range of the family beyond the two-electron oxidation (hydroxylation...Continue Reading

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Citations

Feb 7, 2012·Biochemistry·Laura M K DassamaJ Martin Bollinger
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
Dec 9, 2008·Applied and Environmental Microbiology·Tae Seok MoonKristala L Jones Prather
Aug 2, 2011·Yakugaku zasshi : Journal of the Pharmaceutical Society of Japan·Hajime Hirao, Keiji Morokuma
Apr 18, 2014·PloS One·Lígia S NobreLígia M Saraiva
Aug 8, 2007·Proceedings of the National Academy of Sciences of the United States of America·Carole MathevonMohamed Atta
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
Jun 20, 2015·Journal of the American Chemical Society·Rae Ana SnyderEdward I Solomon
Jan 29, 2009·Dalton Transactions : an International Journal of Inorganic Chemistry·J Martin BollingerCarsten Krebs
Jul 3, 2016·Journal of Biological Inorganic Chemistry : JBIC : a Publication of the Society of Biological Inorganic Chemistry·Edward I Solomon, Kiyoung Park
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