Literature DB >> 21322488

Implications for the mechanism of sulfite oxidizing enzymes from pulsed EPR spectroscopy and DFT calculations for "difficult" nuclei.

John H Enemark1, Arnold M Raitsimring, Andrei V Astashkin, Eric L Klein.   

Abstract

The catalytic mechanisms of sulfite oxidizing enzymes (SOEs) have been investigated by multi-frequency pulsed EPR measurements of "difficult" magnetic nuclei (35.37Cl, 33S, 17O) associated with the Mo(v) center. Extensive DFT calculations have been used to relate the experimental magnetic resonance parameters of these nuclei to specific active site structures. This combined spectroscopic and computational approach has provided new insights concerning the structure/function relationships of the active sites of SOEs, including: (i) the exchange of oxo ligands; (ii) the nature of the blocked forms; and (iii) the role of Cl- in low pH forms.

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Year:  2011        PMID： 21322488      PMCID： PMC3079391          DOI： 10.1039/c004404k

Source DB:  PubMed          Journal:  Faraday Discuss        ISSN： 1359-6640            Impact factor:   4.008


  34 in total

1.  17O ESEEM evidence for exchange of the axial oxo ligand in the molybdenum center of the high pH form of sulfite oxidase.

Authors:  Andrei V Astashkin; Changjian Feng; Arnold M Raitsimring; John H Enemark
Journal:  J Am Chem Soc       Date:  2005-01-19       Impact factor: 15.419

2.  Spectroscopic and kinetic studies of Arabidopsis thaliana sulfite oxidase: nature of the redox-active orbital and electronic structure contributions to catalysis.

Authors:  Craig Hemann; Brian L Hood; Meita Fulton; Robert Hänsch; Günter Schwarz; Ralf R Mendel; Martin L Kirk; Russ Hille
Journal:  J Am Chem Soc       Date:  2005-11-30       Impact factor: 15.419

3.  Structure of the active site of sulfite oxidase. X-ray absorption spectroscopy of the Mo(IV), Mo(V), and Mo(VI) oxidation states.

Authors:  G N George; C A Kipke; R C Prince; R A Sunde; J H Enemark; S P Cramer
Journal:  Biochemistry       Date:  1989-06-13       Impact factor: 3.162

Review 4.  The inorganic biochemistry of molybdoenzymes.

Authors:  R C Bray
Journal:  Q Rev Biophys       Date:  1988-08       Impact factor: 5.318

5.  Identification and biochemical characterization of Arabidopsis thaliana sulfite oxidase. A new player in plant sulfur metabolism.

Authors:  T Eilers; G Schwarz; H Brinkmann; C Witt; T Richter; J Nieder; B Koch; R Hille; R Hänsch; R R Mendel
Journal:  J Biol Chem       Date:  2001-10-11       Impact factor: 5.157

Review 6.  Molybdenum-cofactor-containing enzymes: structure and mechanism.

Authors:  C Kisker; H Schindelin; D C Rees
Journal:  Annu Rev Biochem       Date:  1997       Impact factor: 23.643

7.  Pulsed EPR studies of nonexchangeable protons near the Mo(V) center of sulfite oxidase: direct detection of the alpha-proton of the coordinated cysteinyl residue and structural implications for the active site.

Authors:  Andrei V Astashkin; Arnold M Raitsimring; Changjian Feng; Jean L Johnson; K V Rajagopalan; John H Enemark
Journal:  J Am Chem Soc       Date:  2002-05-29       Impact factor: 15.419

8.  Structural studies of the molybdenum center of the pathogenic R160Q mutant of human sulfite oxidase by pulsed EPR spectroscopy and 17O and 33S labeling.

Authors:  Andrei V Astashkin; Kayunta Johnson-Winters; Eric L Klein; Changjian Feng; Heather L Wilson; K V Rajagopalan; Arnold M Raitsimring; John H Enemark
Journal:  J Am Chem Soc       Date:  2008-06-05       Impact factor: 15.419

9.  Intramolecular electron transfer in sulfite-oxidizing enzymes: elucidating the role of a conserved active site arginine.

Authors:  Safia Emesh; Trevor D Rapson; Asha Rajapakshe; Ulrike Kappler; Paul V Bernhardt; Gordon Tollin; John H Enemark
Journal:  Biochemistry       Date:  2009-03-17       Impact factor: 3.162

10.  Equilibria amongst different molybdenum (V)-containing species from sulphite oxidase. Evidence for a halide ligand of molybdenum in the low-pH species.

Authors:  R C Bray; S Gutteridge; M T Lamy; T Wilkinson
Journal:  Biochem J       Date:  1983-04-01       Impact factor: 3.857
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  7 in total

1.  Applications of pulsed EPR spectroscopy to structural studies of sulfite oxidizing enzymes().

Authors:  Eric L Klein; Andrei V Astashkin; Arnold M Raitsimring; John H Enemark
Journal:  Coord Chem Rev       Date:  2013-01-01       Impact factor: 22.315

Review 2.  The mononuclear molybdenum enzymes.

Authors:  Russ Hille; James Hall; Partha Basu
Journal:  Chem Rev       Date:  2014-01-28       Impact factor: 60.622

3.  Structural studies of the molybdenum center of mitochondrial amidoxime reducing component (mARC) by pulsed EPR spectroscopy and 17O-labeling.

Authors:  Asha Rajapakshe; Andrei V Astashkin; Eric L Klein; Debora Reichmann; Ralf R Mendel; Florian Bittner; John H Enemark
Journal:  Biochemistry       Date:  2011-09-22       Impact factor: 3.162

4.  Identity of the exchangeable sulfur-containing ligand at the Mo(V) center of R160Q human sulfite oxidase.

Authors:  Eric L Klein; Arnold M Raitsimring; Andrei V Astashkin; Asha Rajapakshe; Kayunta Johnson-Winters; Anna R Arnold; Alexey Potapov; Daniella Goldfarb; John H Enemark
Journal:  Inorg Chem       Date:  2012-01-06       Impact factor: 5.165

5.  Characterization of chloride-depleted human sulfite oxidase by electron paramagnetic resonance spectroscopy: experimental evidence for the role of anions in product release.

Authors:  Asha Rajapakshe; Kayunta Johnson-Winters; Anna R Nordstrom; Kimberly T Meyers; Safia Emesh; Andrei V Astashkin; John H Enemark
Journal:  Biochemistry       Date:  2010-06-29       Impact factor: 3.162

Review 6.  Elucidating the catalytic mechanism of sulfite oxidizing enzymes using structural, spectroscopic, and kinetic analyses.

Authors:  Kayunta Johnson-Winters; Gordon Tollin; John H Enemark
Journal:  Biochemistry       Date:  2010-08-31       Impact factor: 3.162

Review 7.  Nitrate and periplasmic nitrate reductases.

Authors:  Courtney Sparacino-Watkins; John F Stolz; Partha Basu
Journal:  Chem Soc Rev       Date:  2014-01-21       Impact factor: 54.564
  7 in total

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