Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 117, Issue 35, Pages 21045-21051Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.2010815117
Keywords
electron bifurcation; electron transfer; short-circuiting; bioenergetics; chemiosmotic hypothesis
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Funding
- Biological Electron Transfer and Catalysis EFRC, an Energy Frontier Research Center - US Department of Energy, Office of Science [DE-SC0012518]
- US Department of Energy (DOE) [DE-AC36-08GO28308]
- US DOE Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, Physical Biosciences Program
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For decades, it was unknown how electron-bifurcating systems in nature prevented energy-wasting short-circuiting reactions that have large driving forces, so synthetic electron-bifurcating molecular machines could not be designed and built. The underpinning free-energy landscapes for electron bifurcation were also enigmatic. We predict that a simple and universal free-energy landscape enables electron bifurcation, and we show that it enables high-efficiency bifurcation with limited short-circuiting (the EB scheme). The landscape relies on steep free-energy slopes in the two redox branches to insulate against short-circuiting using an electron occupancy blockade effect, without relying on nuanced changes in the microscopic rate constants for the short-circuiting reactions. The EB scheme thus unifies a body of observations on biological catalysis and energy conversion, and the scheme provides a blueprint to guide future campaigns to establish synthetic electron bifurcation machines.
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