Asymmetric size of ions and orientational ordering of water dipoles in electric double layer model - an analytical mean-field approach

Gongadze, Ekaterina; Iglič, Aleš

doi:10.1016/j.electacta.2015.07.179

Cited by 79 publications

(122 citation statements)

References 53 publications

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“…Like previous experimental and theoretical studies, our work shows that water adsorbs at the Au(111) surface with increasing absolute potential. In addition, we are able to show that this agglomeration of water has an influence on the C DL, the main signature is the increase in C DL at potentials positive of the pzc .…”

Section: Discussionsupporting

confidence: 87%

“…Impedance spectra were obtained, which could be modeled with two equivalent circuits.T he C DL versus potential curves for the various water contentsw ere comparedw ithaprediction madeb ym eanfield theory. [23] Like previous experimental [13,14] and theoretical studies, [10][11][12] our work shows that water adsorbs at the Au(111)s urfacew ith increasing absolute potential. In addition, we are able to show that this agglomeration of water has an influence on the C DL, [10] the main signature is the increase in C DL at potentials positive of the pzc.…”

Section: Discussionsupporting

confidence: 82%

“…Like our present simple estimate, as described in the SupportingI nformation, the BKK model does not take into account possible "freezing" of orientational polarizability of solvent dipoles;t heir model is better applicable for nonpolars olvent additives. Gongadze and Iglič [12] developed another mean-field model, in which the dielectric saturation of solvent molecules with permanent dipole moments has been explicitly considered, but these have not been studied in detail and, most importantly,t he results for ca-pacitance have not been displayed. It might be interesting to combine the two approaches in an attempt to integrate the dielectric saturation effect into an extended version of the BKK model.…”

Section: ) Ar Esistor (R Ohm )I Ns Eries To Ac Apacitor (C Hf )A Nd mentioning

confidence: 99%

“…The adsorption of water at electrodes has only recently been studied theoretically and experimentally . Feng et al.…”

Section: Introductionmentioning

confidence: 99%

“…[4À7] Waterw as found to exist mostly as monomers, often trapped closet o hydrophilic moieties. [8,9] The adsorption of water at electrodes has only recently been studied theoretically [10][11][12] and experimentally. [13,14] Feng et al studied humid imidazolium-based ionic liquidsa nd the adsorption of water at ac arbon-like electrode using molecular dynamics simulations.…”

Section: Introductionmentioning

confidence: 99%

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Interface between an Au(111) Surface and an Ionic Liquid: The Influence of Water on the Double‐Layer Capacitance

Friedl

Markovits²,

Herpich³

et al. 2016

ChemElectroChem

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The presence of water in room‐temperature ionic liquids (RTILs) can have a strong effect on their properties. In particular, water adsorption at electrodes can reduce the electrochemical potential window of the system. It is, thus, important to understand where water will be present depending on the electrode potential, the type of ionic liquid, and the electrode material. We investigate the influence of water on RTILs by measuring the potential‐dependent double‐layer capacitance of various water–RTIL mixtures. The resulting capacitance versus potential curves are reproduced employing mean‐field theory calculations. From the parameters used to obtain the best agreement between experimental and theoretical curves, some properties of the RTILs can be deducted, such as a stronger interaction of water with RTIL anions than cations and an agglomeration of water at potentials positive or negative of the potential of zero charge.

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Section: Discussionsupporting

confidence: 87%

Section: Discussionsupporting

confidence: 82%

Section: ) Ar Esistor (R Ohm )I Ns Eries To Ac Apacitor (C Hf )A Nd mentioning

confidence: 99%

“…The adsorption of water at electrodes has only recently been studied theoretically and experimentally . Feng et al.…”

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Interface between an Au(111) Surface and an Ionic Liquid: The Influence of Water on the Double‐Layer Capacitance

Friedl

Markovits²,

Herpich³

et al. 2016

ChemElectroChem

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Understanding the Electric Double Layer at the Electrode‐Electrolyte Interface: Part I – No Ion Specific Adsorption

Mazur,

Brandyshev,

Doronin

et al. 2024

ChemPhysChem

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We present a comprehensive mean‐field model that takes into account the key components of modern electrical double layer theory at the interface between an electrode and an electrolyte solution. The model considers short‐range specific interactions between different species, including electrode‐ion repulsion, the hydration of ions, dielectric saturation of solvent (water), and excluded volume (steric) interactions between species. By solving a modified Poisson‐Boltzmann equation and using the appropriate results of quantum chemistry calculations on the hydration of ions, we can accurately approximate the differential capacitance profiles of aqueous electrolyte solutions at the boundary with a silver electrode. The specific interactions between the ions and the electrodes in the systems under consideration are assumed to be significantly weaker than their Coulomb interactions. A novel aspect of our research is the investigation of the impact of short‐range ion‐water interactions on the differential capacitance, which provides new insights into the behavior of the electrical double layer. This model holds the potential to be useful for electrochemical engineers working on the development of supercapacitors and related electrochemical energy storage devices. It serves as a basis for future modeling of electrolyte systems on real electrodes, especially in scenarios where chemical ion‐electrode interactions are significant.

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Elementary Concepts and Definitions

Brosseau

2023

Studies in Mechanobiology, Tissue Engineering and Biomaterials

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Asymmetric size of ions and orientational ordering of water dipoles in electric double layer model - an analytical mean-field approach

Cited by 79 publications

References 53 publications

Interface between an Au(111) Surface and an Ionic Liquid: The Influence of Water on the Double‐Layer Capacitance

Interface between an Au(111) Surface and an Ionic Liquid: The Influence of Water on the Double‐Layer Capacitance

Understanding the Electric Double Layer at the Electrode‐Electrolyte Interface: Part I – No Ion Specific Adsorption

Elementary Concepts and Definitions

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