Intramolecular electron transfer in Pseudomonas aeruginosa cd(1) nitrite reductase: thermodynamics and kinetics.

Biophysical Journal
O FarverI Pecht

Abstract

The cd(1) nitrite reductases, which catalyze the reduction of nitrite to nitric oxide, are homodimers of 60 kDa subunits, each containing one heme-c and one heme-d(1). Heme-c is the electron entry site, whereas heme-d(1) constitutes the catalytic center. The 3D structure of Pseudomonas aeruginosa nitrite reductase has been determined in both fully oxidized and reduced states. Intramolecular electron transfer (ET), between c and d(1) hemes is an essential step in the catalytic cycle. In earlier studies of the Pseudomonas stutzeri enzyme, we observed that a marked negative cooperativity is controlling this internal ET step. In this study we have investigated the internal ET in the wild-type and His369Ala mutant of P. aeruginosa nitrite reductases and have observed similar cooperativity to that of the Pseudomonas stutzeri enzyme. Heme-c was initially reduced, in an essentially diffusion-controlled bimolecular process, followed by unimolecular electron equilibration between the c and d(1) hemes (k(ET) = 4.3 s(-1) and K = 1.4 at 298 K, pH 7.0). In the case of the mutant, the latter ET rate was faster by almost one order of magnitude. Moreover, the internal ET rate dropped (by approximately 30-fold) as the level of reduction increase...Continue Reading

References

Feb 28, 2001·Proceedings of the National Academy of Sciences of the United States of America·F CutruzzolaM Brunori
May 25, 2001·The Journal of Biological Chemistry·T Sjögren, J Hajdu
Sep 21, 2001·Journal of Molecular Biology·K BrownM Tegoni
Feb 7, 2002·Biochemical and Biophysical Research Communications·Wenliang SunFrancesca Cutruzzolà
Jun 13, 2003·Proceedings of the National Academy of Sciences of the United States of America·Ole FarverIsrael Pecht
Mar 20, 2004·Quarterly Reviews of Biophysics·Harry B Gray, Jay R Winkler

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Citations

Jun 26, 2009·BioEssays : News and Reviews in Molecular, Cellular and Developmental Biology·Francesca CutruzzolàMaurizio Brunori
Aug 15, 2014·Biochemical and Biophysical Research Communications·Serena RinaldoFrancesca Cutruzzolà
Jan 27, 2011·Biochemical Society Transactions·Serena RinaldoFrancesca Cutruzzolà
Apr 4, 2014·Chemical Reviews·Luisa B Maia, José J G Moura
Feb 24, 2016·Journal of Bacteriology·José Manuel Borrero-de AcuñaDieter Jahn
Apr 8, 2020·The FEBS Journal·Thomas KlünemannWulf Blankenfeldt
Jun 9, 2020·Acta Crystallographica. Section F, Structural Biology Communications·Thomas Klünemann, Wulf Blankenfeldt
Dec 9, 2009·Journal of the American Chemical Society·Ole FarverIsrael Pecht
Feb 12, 2019·Chemical Reviews·Kazuo Kobayashi

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