Gelation, clustering, and crowding in the electrical double layer of ionic liquids

Gelation, clustering, and crowding in the electrical double layer of ionic liquids

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. [J. Phys. Chem. B 125, 2677 (2021)] developed a t...

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Veröffentlicht in:The Journal of chemical physics 2022-09, Vol.157 (9), p.094106-094106
Hauptverfasser: Goodwin, Zachary A. H., McEldrew, Michael, Pedro de Souza, J., Bazant, Martin Z., Kornyshev, Alexei A.
Format: Artikel
Sprache:eng
Schlagworte:
Clustering
Crowding
Electric double layer
Electrolytes
Gelation
Interfacial properties
Ionic liquids
Percolation
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container_end_page 094106
container_issue 9
container_start_page 094106
container_title The Journal of chemical physics
container_volume 157
creator Goodwin, Zachary A. H.
McEldrew, Michael
Pedro de Souza, J.
Bazant, Martin Z.
Kornyshev, Alexei A.
description 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. [J. Phys. Chem. B 125, 2677 (2021)] 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 crowding regime dominated by free ions. This transition from gelation to crowding is conceptually similar to the overscreening to crowding transition.
doi_str_mv 10.1063/5.0097055
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source AIP Journals Complete; Alma/SFX Local Collection
subjects Clustering
Crowding
Electric double layer
Electrolytes
Gelation
Interfacial properties
Ionic liquids
Percolation
title Gelation, clustering, and crowding in the electrical double layer of ionic liquids
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