Publications [#351428] of David N. Beratan

Journal Articles

1. Yuly, JL; Zhang, P; Lubner, CE; Peters, JW; Beratan, DN, Universal free-energy landscape produces efficient and reversible electron bifurcation., Proceedings of the National Academy of Sciences of the United States of America, vol. 117 no. 35 (September, 2020), pp. 21045-21051 [doi]
   (last updated on 2025/07/06)

   Abstract:
   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.