Theory of Ionic Liquids with Polarizable Ions on a Charged Electrode,The Journal of Physical Chemistry C

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Theory of Ionic Liquids with Polarizable Ions on a Charged Electrode
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2021-09-15 , DOI: 10.1021/acs.jpcc.1c05548
Yury A. Budkov _{1,

2} , Semen V. Zavarzin ₁ , Andrei L. Kolesnikov ₃

Affiliation

We formulate a general mean-field theory for a flat electric double layer in ionic liquids and electrolyte solutions with ions possessing static polarizability and a permanent dipole moment on a charged electrode. We establish a new analytical expression for electric double-layer differential capacitance, determining it as an absolute value of the ratio of the local ionic charge density to the local electric field on an electrode surface. We demonstrate that this expression generalizes the analytical expressions previously reported by Kornyshev and Maggs and Podgornik. Using the obtained analytical expression, we explore new features of the differential capacitance behavior with an increase in the static polarizability and permanent dipole moment of cations. We relate these features to the behavior of ionic concentrations on the electrode. In particular, we elucidate the role of the competition between the dielectrophoretic attraction and Coulomb repulsion forces acting on polarizable or polar cations in the electric double layer in the behavior of the differential capacitance. The developed theoretical model and obtained theoretical findings could be relevant for different electrochemical applications, e.g., batteries, supercapacitors, catalysis, electrodeposition, etc.

中文翻译：

带电电极上具有可极化离子的离子液体理论

我们为离子液体和电解质溶液中的平面双电层制定了一般平均场理论，其中离子在带电电极上具有静态极化性和永久偶极矩。我们建立了双电层微分电容的新解析表达式，将其确定为电极表面上局部离子电荷密度与局部电场之比的绝对值。我们证明该表达式概括了 Kornyshev 和 Maggs 以及 Podgornik 先前报告的分析表达式。使用获得的解析表达式，我们探索了随着阳离子的静态极化率和永久偶极矩的增加，差分电容行为的新特征。我们将这些特征与电极上离子浓度的行为联系起来。特别地，我们阐明了介电泳吸引力和库仑排斥力之间的竞争作用在微分电容行为中的双电层中的可极化或极性阳离子上。开发的理论模型和获得的理论发现可能与不同的电化学应用相关，例如电池、超级电容器、催化、电沉积等。

更新日期：2021-09-30

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