<br>将双电层形成与电催化活性联系起来,ACS Catalysis

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将双电层形成与电催化活性联系起来
ACS Catalysis ( IF 11.3 ) Pub Date : 2023-12-05 , DOI: 10.1021/acscatal.3c04255
Matthew A. Gebbie ₁ , Beichen Liu ₁ , Wenxiao Guo ₁ , Seth R. Anderson ₁ , Samuel G. Johnstone ₁

Affiliation

双电层在电极-电解质界面形成，通常在控制电化学反应速率和选择性方面发挥决定性作用。虽然一个多世纪以来双层形成一直是一个活跃的研究领域，但大多数用于预测双电层特性的框架，例如局部离子浓度、电势梯度和反应物化学势，仍然植根于经典的古伊-查普曼-斯特恩模型理论，该理论忽略了离子-离子相互作用并假设非反应性界面。然而，表面力和电催化领域的最新发现强调了离子-离子相互作用的出现如何从根本上改变双电层形成机制和界面特性。值得注意的是，最近对离子液体的研究表明，离子关联和聚集可以显着改变反应速率和选择性，特别是在浓电解质中。此外，新兴研究表明，电双层结构和动力学在发生电催化反应的电位下会发生显着变化。在这里，我们提供了关于离子-离子相互作用如何影响双电层特性并有助于调节电催化系统的观点，特别是在高离子浓度和大施加电势导致偏离经典电解质理论的条件下。我们还总结了越来越多的问题和机会，以进一步探索电化学反应如何彻底改变双电层特性。我们总结了这些发现如何为利用电催化反应研究双电层形成并通过设计电极-电解质界面实现电化学转换打开了大门。

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Linking Electric Double Layer Formation to Electrocatalytic Activity

Electric double layers form at electrode–electrolyte interfaces and often play defining roles in governing electrochemical reaction rates and selectivity. While double layer formation has remained an active area of research for more than a century, most frameworks used to predict electric double layer properties, such as local ion concentrations, potential gradients, and reactant chemical potentials, remain rooted in classical Gouy–Chapman–Stern theory, which neglects ion–ion interactions and assumes nonreactive interfaces. Yet, recent findings from the surface forces and electrocatalysis communities have highlighted how the emergence of ion–ion interactions fundamentally alters electric double layer formation mechanisms and interface properties. Notably, recent studies with ionic liquids show that ionic correlations and clustering can substantially alter reaction rates and selectivity, especially in concentrated electrolytes. Further, emerging studies suggest that electric double layer structures and dynamics significantly change at potentials where electrocatalytic reactions occur. Here, we provide our perspective on how ion–ion interactions can impact electric double layer properties and contribute to modulating electrocatalytic systems, especially under conditions where high ion concentrations and large applied potentials cause deviations from classical electrolyte theory. We also summarize growing questions and opportunities to further explore how electrochemical reactions can drastically alter electric double layer properties. We conclude with a perspective on how these findings open the door to using electrocatalytic reactions to study electric double layer formation and achieve electrochemical conversion by engineering electrode–electrolyte interfaces.

更新日期：2023-12-05

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