Pathways for proton release during ubihydroquinone oxidation by the bc 1 complex
10.1073/pnas.96.18.10021
Crossref journal-article
Proceedings of the National Academy of Sciences
Proceedings of the National Academy of Sciences (341)
Abstract

Quinol oxidation by the bc 1 complex of Rhodobacter sphaeroides occurs from an enzyme–substrate complex formed between quinol bound at the Q o site and the iron–sulfur protein (ISP) docked at an interface on cytochrome b . From the structure of the stigmatellin-containing mitochondrial complex, we suggest that hydrogen bonds to the two quinol hydroxyl groups, from Glu-272 of cytochrome b and His-161 of the ISP, help to stabilize the enzyme–substrate complex and aid proton release. Reduction of the oxidized ISP involves H transfer from quinol. Release of the proton occurs when the acceptor chain reoxidizes the reduced ISP, after domain movement to an interface on cytochrome c 1 . Effects of mutations to the ISP that change the redox potential and/or the pK on the oxidized form support this mechanism. Structures for the complex in the presence of inhibitors show two different orientations of Glu-272. In stigmatellin-containing crystals, the side chain points into the site, to hydrogen bond with a ring hydroxyl, while His-161 hydrogen bonds to the carbonyl group. In the native structure, or crystals containing myxothiazol or β-methoxyacrylate-type inhibitors, the Glu-272 side chain is rotated to point out of the site, to the surface of an external aqueous channel. Effects of mutation at this residue suggest that this group is involved in ligation of stigmatellin and quinol, but not quinone, and that the carboxylate function is essential for rapid turnover. H + transfer from semiquinone to the carboxylate side chain and rotation to the position found in the myxothiazol structure provide a pathway for release of the second proton.

Bibliography

Crofts, A. R., Hong, S., Ugulava, N., Barquera, B., Gennis, R., Guergova-Kuras, M., & Berry, E. A. (1999). Pathways for proton release during ubihydroquinone oxidation by the bc 1 complex. Proceedings of the National Academy of Sciences, 96(18), 10021–10026.

Authors 7
  1. Antony R. Crofts (first)
  2. Sangjin Hong (additional)
  3. Natalia Ugulava (additional)
  4. Blanca Barquera (additional)
  5. Robert Gennis (additional)
  6. Mariana Guergova-Kuras (additional)
  7. Edward A. Berry (additional)
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Dates
Type When
Created 23 years, 1 month ago (July 26, 2002, 6:38 a.m.)
Deposited 3 years, 2 months ago (June 6, 2022, 8:35 p.m.)
Indexed 4 weeks, 2 days ago (Aug. 6, 2025, 8:29 a.m.)
Issued 26 years ago (Aug. 31, 1999)
Published 26 years ago (Aug. 31, 1999)
Published Online 26 years ago (Aug. 31, 1999)
Published Print 26 years ago (Aug. 31, 1999)
Funders 0

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@article{Crofts_1999, title={Pathways for proton release during ubihydroquinone oxidation by the bc 1 complex}, volume={96}, ISSN={1091-6490}, url={http://dx.doi.org/10.1073/pnas.96.18.10021}, DOI={10.1073/pnas.96.18.10021}, number={18}, journal={Proceedings of the National Academy of Sciences}, publisher={Proceedings of the National Academy of Sciences}, author={Crofts, Antony R. and Hong, Sangjin and Ugulava, Natalia and Barquera, Blanca and Gennis, Robert and Guergova-Kuras, Mariana and Berry, Edward A.}, year={1999}, month=aug, pages={10021–10026} }