Mechanistic insights into energy conservation by flavin-based electron bifurcation

Carolyn E. Lubner; David P. Jennings; David W. Mulder; Gerrit J. Schut; Oleg A. Zadvornyy; John P. Hoben; Monika Tokmina-Lukaszewska; Luke Berry; Diep M. Nguyen; Gina L. Lipscomb; Brian Bothner; Anne Jones; Anne Frances Miller; Paul W. King; Michael W.W. Adams; John W. Peters

doi:10.1038/nchembio.2348

Mechanistic insights into energy conservation by flavin-based electron bifurcation

Carolyn E. Lubner, David P. Jennings, David W. Mulder, Gerrit J. Schut, Oleg A. Zadvornyy, John P. Hoben, Monika Tokmina-Lukaszewska, Luke Berry, Diep M. Nguyen, Gina L. Lipscomb, Brian Bothner, Anne Jones, Anne Frances Miller, Paul W. King, Michael W.W. Adams, John W. Peters

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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. 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.

Original language	English (US)
Pages (from-to)	655-659
Number of pages	5
Journal	Nature Chemical Biology
Volume	13
Issue number	6
DOIs	https://doi.org/10.1038/nchembio.2348
State	Published - Jun 1 2017

ASJC Scopus subject areas

Molecular Biology
Cell Biology

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10.1038/nchembio.2348

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Lubner, C. E., Jennings, D. P., Mulder, D. W., Schut, G. J., Zadvornyy, O. A., Hoben, J. P., Tokmina-Lukaszewska, M., Berry, L., Nguyen, D. M., Lipscomb, G. L., Bothner, B., Jones, A., Miller, A. F., King, P. W., Adams, M. W. W., & Peters, J. W. (2017). Mechanistic insights into energy conservation by flavin-based electron bifurcation. Nature Chemical Biology, 13(6), 655-659. https://doi.org/10.1038/nchembio.2348

Lubner, CE, Jennings, DP, Mulder, DW, Schut, GJ, Zadvornyy, OA, Hoben, JP, Tokmina-Lukaszewska, M, Berry, L, Nguyen, DM, Lipscomb, GL, Bothner, B, Jones, A, Miller, AF, King, PW, Adams, MWW & Peters, JW 2017, 'Mechanistic insights into energy conservation by flavin-based electron bifurcation', Nature Chemical Biology, vol. 13, no. 6, pp. 655-659. https://doi.org/10.1038/nchembio.2348

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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. 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.",

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AU - Nguyen, Diep M.

AU - Lipscomb, Gina L.

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AB - 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. 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.

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Mechanistic insights into energy conservation by flavin-based electron bifurcation

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NADH-dependent Ferredoxin:NADP Oxidoreductase (NfnI) from Pyrococcus furiosus

NADP(H) bound NADH-dependent Ferredoxin:NADP Oxidoreductase (NfnI) from Pyrococcus furiosus

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Mechanistic insights into energy conservation by flavin-based electron bifurcation

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ASJC Scopus subject areas

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NADH-dependent Ferredoxin:NADP Oxidoreductase (NfnI) from Pyrococcus furiosus

NADP(H) bound NADH-dependent Ferredoxin:NADP Oxidoreductase (NfnI) from Pyrococcus furiosus

Cite this