普适自由能景观产生有效和可逆的电子分叉
Universal Free Energy Landscape Produces Efficient and Reversible Electron Bifurcation
摘要：
几十年来，人们不知道自然界中的电子分叉系统如何防止具有大驱动力的能量浪费短路反应，因此无法设计和建造合成电子分叉分子机器。支撑电子分叉的自由能景观也是谜。我们预测，一个简单的和普遍的自由能景观使电子分叉，我们表明，它使高效率的分叉有限的短路（EB计划）。景观依赖于两个氧化还原分支中陡峭的自由能斜率来隔离短路，而不依赖于短路反应微观速率常数的细微变化。因此，EB计划为未来建立合成电子分叉机的运动提供了蓝图。
英文摘要：
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 without relying on nuanced changes in the microscopic rate constants for the short-circuiting reactions. The EB-scheme thus provides a blueprint for future campaigns to establish synthetic electron bifurcating machines.
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