Mean-Field Theory of the Electrical Double Layer in Ionic Liquids

Goodwin, Zachary A. H.; Souza, J. Pedro de; Bazant, Martin Z.; Kornyshev, Alexei A.

doi:10.1007/978-981-10-6739-6_62-1

Cited by 9 publications

(13 citation statements)

References 57 publications

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“…The presented theory could be considered to overestimate the extent of clusters in the EDL, then. Therefore, it is expected that the cluster distribution in the EDL does not exactly hold, but we believe it is a sufficiently good approximation to understand the qualitative behaviour, as is evident from its predictions which are qualitatively consistent with a large body of literature [3,77].…”

Section: Assumptions Of the Theorysupporting

confidence: 74%

“…The theory of McEldrew et al [60] was applied to bulk ILs [61], and other concentrated electrolytes [62,63], where a consistent theory of ionic transport was also developed based on vehicular motion of the clusters [61,76]. While the ionic association theory has given a detailed description of the cluster statistics in the bulk, it has not yet been applied to predict the distributions of clusters near charged interfaces in the electrical double layer (EDL) [77].…”

Section: Introductionmentioning

confidence: 99%

“…If a "standard approach" is taken for the EDL-Bulk equilibrium, i.e. where the ions in the bulk are assumed to accumulate in the EDL based on a Poisson-Boltzmann or Poisson-Fermi distribution from the bulk concentrations [77][78][79][80], the ions are not permitted to reversibly associate in the EDL [49,[52][53][54]. Such approaches bring ions to the EDL based on the charge and volume of the ion, but once the species are in the EDL, no further change of the ionic associations can occur.…”

Section: Introductionmentioning

confidence: 99%

“…Alternatively, an approach similar to how solvent is treated in the dilute electrolyte limit could be taken, i.e. the gel can be taken as some constant background dielectric, which would be trivially pushed out of the EDL based on how ions come to the EDL [77,80].…”

Section: Introductionmentioning

confidence: 99%

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Gelation, Clustering and Crowding in the Electrical Double Layer of Ionic Liquids

Goodwin,

McEldrew,

de Souza

et al. 2022

Preprint

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Understanding the bulk and interfacial properties of super-concentrated electrolytes, such as ionic liquids (ILs), has attracted significant attention lately for their promising applications in supercapacitors and batteries. Recently, McEldrew et al. developed a theory for reversible ion associations in bulk ILs, which accounted for the formation of all possible Cayley tree clusters and a percolating ionic network (gel). Here we adopt and develop this approach to understand the associations of ILs in the electrical double layer at electrified interfaces. With increasing charge of the electrode, the theory predicts a transition from a regime dominated by a gelled or clustered state to a regime dominated by free, crowded ions. This transition from gelation to crowding is conceptually similar to the overscreening to crowding transition.

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Section: Assumptions Of the Theorysupporting

confidence: 74%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Gelation, Clustering and Crowding in the Electrical Double Layer of Ionic Liquids

Goodwin,

McEldrew,

de Souza

et al. 2022

Preprint

Self Cite

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“…It is complementary to previous reviews on this topic, which rather focused on electrostatic models for the simulation of electrode− solution interfaces 43 or the use of mean-field theories. 44 Another review was devoted to the molecular simulations of capacitive energy storage devices. 45 However, the field has remained very active during the past five years, and the present review also accounts for these latest developments.…”

Section: Introductionmentioning

confidence: 99%

Microscopic Simulations of Electrochemical Double-Layer Capacitors

2022

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Electrochemical double-layer capacitors (EDLCs) are devices allowing the storage or production of electricity. They function through the adsorption of ions from an electrolyte on high-surface-area electrodes and are characterized by short charging/ discharging times and long cycle-life compared to batteries. Microscopic simulations are now widely used to characterize the structural, dynamical, and adsorption properties of these devices, complementing electrochemical experiments and in situ spectroscopic analyses. In this review, we discuss the main families of simulation methods that have been developed and their application to the main family of EDLCs, which include nanoporous carbon electrodes. We focus on the adsorption of organic ions for electricity storage applications as well as aqueous systems in the context of blue energy harvesting and desalination. We finally provide perspectives for further improvement of the predictive power of simulations, in particular for future devices with complex electrode compositions.

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Size polydisperse model ionic liquid under confinement: A molecular dynamics study

Urikhinbam,

Shagolsem

2024

Journal of Molecular Liquids

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Mean-Field Theory of the Electrical Double Layer in Ionic Liquids

Cited by 9 publications

References 57 publications

Gelation, Clustering and Crowding in the Electrical Double Layer of Ionic Liquids

Gelation, Clustering and Crowding in the Electrical Double Layer of Ionic Liquids

Microscopic Simulations of Electrochemical Double-Layer Capacitors

Size polydisperse model ionic liquid under confinement: A molecular dynamics study

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