论文标题

通过电子传输反应调整电化学界面的稳定性

Tuning the stability of Electrochemical Interfaces by Electron Transfer reactions

论文作者

Fraggedakis, Dimitrios, Bazant, Martin Z.

论文摘要

已知界面的形态在与能量相关的应用,这样的光收集或离子插入的效率上起着基本作用。但是,按需改变形态是一项非常艰巨的任务。在这里,我们展示了界面的形态可以通过驱动的电子传递反应来调节。通过使用非平衡热力学稳定性理论,我们发现了改变界面形态的工作条件。我们将理论应用于离子插入和表面生长,其中使用Butler-volmer或耦合的离子 - 电子转移动力学描述了电化学反应。后者将微观/量子机械概念与电化学界面的形态联系起来。最后,我们根据所施加的驱动力(电流/电压)构建非平衡相图,并讨论电子供体状态在与能量收集和存储,电催化和光催化有关的应用中的重要性。

The morphology of interfaces is known to play fundamental role on the efficiency of energy-related applications, such light harvesting or ion intercalation. Altering the morphology on demand, however, is a very difficult task. Here, we show ways the morphology of interfaces can be tuned by driven electron transfer reactions. By using non-equilibrium thermodynamic stability theory, we uncover the operating conditions that alter the interfacial morphology. We apply the theory to ion intercalation and surface growth where electrochemical reactions are described using Butler-Volmer or coupled ion-electron transfer kinetics. The latter connects microscopic/quantum mechanical concepts with the morphology of electrochemical interfaces. Finally, we construct non-equilibrium phase diagrams in terms of the applied driving force (current/voltage) and discuss the importance of engineering the density of states of the electron donor in applications related to energy harvesting and storage, electrocatalysis and photocatalysis.

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