Mechanistic insights into energy conservation by flavin-based electron bifurcation
Abstract
The recently realized biochemical phenomenon of energy conservation through electron bifurcation provides biology with an elegant means to maximize utilization of metabolic energy. The mechanism of coordinated coupling of exergonic and endergonic oxidation-reduction reactions by a single enzyme complex has been elucidated through optical and paramagnetic spectroscopic studies revealing unprecedented features. Pairs of electrons are bifurcated over more than 1 volt of electrochemical potential by generating a low-potential, highly energetic, unstable flavin semiquinone and directing electron flow to an iron-sulfur cluster with a highly negative potential to overcome the barrier of the endergonic half reaction. As a result, the unprecedented range of thermodynamic driving force that is generated by flavin-based electron bifurcation accounts for unique chemical reactions that are catalyzed by these enzymes.
- Authors:
-
[5];
[1];
- National Renewable Energy Lab. (NREL), Golden, CO (United States)
- Arizona State Univ., Tempe, AZ (United States)
- Univ. of Georgia, Athens, GA (United States)
- Montana State Univ., Bozeman, MT (United States)
- Univ. of Kentucky, Lexington, KY (United States)
- Montana State Univ., Bozeman, MT (United States); Washington State Univ., Pullman, WA (United States)
- Publication Date:
- Research Org.:
- National Renewable Energy Laboratory (NREL), Golden, CO (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1358334
- Report Number(s):
- NREL/JA-2700-67530
Journal ID: ISSN 1552-4450
- Grant/Contract Number:
- AC36-08GO28308
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Chemical Biology
- Additional Journal Information:
- Journal Volume: 13; Journal Issue: 6; Journal ID: ISSN 1552-4450
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 09 BIOMASS FUELS; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; structural analysis; spectroscopy; electron bifurcation; flavoenzymes
Citation Formats
Lubner, Carolyn E., Jennings, David P., Mulder, David W., Schut, Gerrit J., Zadvornyy, Oleg A., Hoben, John P., Tokmina-Lukaszewska, Monika, Berry, Luke, Nguyen, Diep M., Lipscomb, Gina L., Bothner, Brian, Jones, Anne K., Miller, Anne-Frances, King, Paul W., Adams, Michael W. W., and Peters, John W. Mechanistic insights into energy conservation by flavin-based electron bifurcation. United States: N. p., 2017.
Web. doi:10.1038/nchembio.2348.
Lubner, Carolyn E., Jennings, David P., Mulder, David W., Schut, Gerrit J., Zadvornyy, Oleg A., Hoben, John P., Tokmina-Lukaszewska, Monika, Berry, Luke, Nguyen, Diep M., Lipscomb, Gina L., Bothner, Brian, Jones, Anne K., Miller, Anne-Frances, King, Paul W., Adams, Michael W. W., & Peters, John W. Mechanistic insights into energy conservation by flavin-based electron bifurcation. United States. https://doi.org/10.1038/nchembio.2348
Lubner, Carolyn E., Jennings, David P., Mulder, David W., Schut, Gerrit J., Zadvornyy, Oleg A., Hoben, John P., Tokmina-Lukaszewska, Monika, Berry, Luke, Nguyen, Diep M., Lipscomb, Gina L., Bothner, Brian, Jones, Anne K., Miller, Anne-Frances, King, Paul W., Adams, Michael W. W., and Peters, John W. Mon .
"Mechanistic insights into energy conservation by flavin-based electron bifurcation". United States. https://doi.org/10.1038/nchembio.2348. https://www.osti.gov/servlets/purl/1358334.
@article{osti_1358334,
title = {Mechanistic insights into energy conservation by flavin-based electron bifurcation},
author = {Lubner, Carolyn E. and Jennings, David P. and Mulder, David W. and Schut, Gerrit J. and Zadvornyy, Oleg A. and Hoben, John P. and Tokmina-Lukaszewska, Monika and Berry, Luke and Nguyen, Diep M. and Lipscomb, Gina L. and Bothner, Brian and Jones, Anne K. and Miller, Anne-Frances and King, Paul W. and Adams, Michael W. W. and Peters, John W.},
abstractNote = {The recently realized biochemical phenomenon of energy conservation through electron bifurcation provides biology with an elegant means to maximize utilization of metabolic energy. The mechanism of coordinated coupling of exergonic and endergonic oxidation-reduction reactions by a single enzyme complex has been elucidated through optical and paramagnetic spectroscopic studies revealing unprecedented features. Pairs of electrons are bifurcated over more than 1 volt of electrochemical potential by generating a low-potential, highly energetic, unstable flavin semiquinone and directing electron flow to an iron-sulfur cluster with a highly negative potential to overcome the barrier of the endergonic half reaction. As a result, the unprecedented range of thermodynamic driving force that is generated by flavin-based electron bifurcation accounts for unique chemical reactions that are catalyzed by these enzymes.},
doi = {10.1038/nchembio.2348},
journal = {Nature Chemical Biology},
number = 6,
volume = 13,
place = {United States},
year = {Mon Apr 10 00:00:00 EDT 2017},
month = {Mon Apr 10 00:00:00 EDT 2017}
}
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