论文标题
通用自由能景观可产生有效且可逆的电子分叉
Universal Free Energy Landscape Produces Efficient and Reversible Electron Bifurcation
论文作者
论文摘要
几十年来，尚不清楚自然界中的电子分叉系统如何阻止具有较大驱动力的短路反应，因此无法设计和构建合成电子分叉分子机。电子分叉的基础自由能景观也是神秘的。我们预测，简单而通用的自由能景观可以实现电子分叉，并且我们表明它可以在有限的短路（EB-Scheme）中实现高效分叉。景观依赖于两个氧化还原分支中的陡峭自由能斜率，以防止短路隔离，而无需依赖于短路反应的微观速率常数变化。因此，EB-Scheme为未来的运动提供了蓝图，以建立合成电子分叉机器。
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.
