Issue 31, 2009
From the journal:

Physical Chemistry Chemical Physics

Exchangeable oxygens in the vicinity of the molybdenum center of the high-pH form of sulfite oxidase and sulfite dehydrogenase†

Andrei V. Astashkin,*a   Eric L. Klein,a   Dmitry Ganyushin,b   Kayunta Johnson-Winters,a   Frank Neese,b   Ulrike Kapplerc  and  John H. Enemarka  

* Corresponding authors

a Department of Chemistry, University of Arizona, Tucson, USA
E-mail: andrei@u.arizona.edu
Fax: +1 (1)520 6218407
Tel: +1 (1)520 6219968

b Institut für Physikalische und Theoretische Chemie, Universität Bonn, Wegelerstrasse 12, 53115 Bonn, Germany
E-mail: neese@thch.uni-bonn.de
Fax: +49 (0)228 739064
Tel: +49 28 732351

c Centre for Metals in Biology, University of Queensland, St. Lucia, Queensland 4072, Australia
E-mail: u.kappler1@uq.edu.au
Fax: +61 (07)3365 4620
Tel: +61 (07)3365 2978

Abstract

The electron spin echo envelope modulation (ESEEM) investigation of the high-pH (hpH) form of sulfite oxidase (SO) and sulfite dehydrogenase (SDH) prepared in buffer enriched with H217O reveals the presence of three types of exchangeable oxygen atoms at the molybdenum center. Two of these oxygen atoms belong to the equatorial OH ligand and the axial oxo ligand, and are characterized by 17O hyperfine interaction (hfi) constants of about 37 MHz and 6 MHz, respectively. The third oxygen has an isotropic hfi constant of 3–4 MHz and likely belongs to a hydroxyl moiety hydrogen-bonded to the equatorial OH ligand. This exchangeable oxygen atom is not observed in the ESEEM spectra of the Y236F mutant of SDH, where the active site tyrosine has been replaced by phenylalanine.

Graphical abstract: Exchangeable oxygens in the vicinity of the molybdenum center of the high-pH form of sulfite oxidase and sulfite dehydrogenase

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Article information

DOI
https://doi.org/10.1039/B907029J
Article type
Paper
Submitted
06 Apr 2009
Accepted
29 Jun 2009
First published
13 Jul 2009

Phys. Chem. Chem. Phys., 2009,11, 6733-6742

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Exchangeable oxygens in the vicinity of the molybdenum center of the high-pH form of sulfite oxidase and sulfite dehydrogenase

A. V. Astashkin, E. L. Klein, D. Ganyushin, K. Johnson-Winters, F. Neese, U. Kappler and J. H. Enemark, Phys. Chem. Chem. Phys., 2009, 11, 6733 DOI: 10.1039/B907029J

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