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

被引：13

作者：

Goodwin, Zachary A. H. ^{[1
,2
]}

McEldrew, Michael ^{[3
]}

de Souza, J. Pedro ^{[3
]}

Bazant, Martin Z. Z. ^{[3
,4
]}

Kornyshev, Alexei A. A. ^{[1
,2
,5
]}

机构：

[1] Imperial Coll London, Dept Chem, Mol Sci Res Hub, White City Campus,Wood Lane, London W12 0BZ, England

[2] Imperial Coll London, Thomas Young Ctr Theory & Simulat Mat, South Kensington Campus, London SW7 2AZ, England

[3] MIT, Dept Chem Engn, Cambridge, MA 02142 USA

[4] MIT, Dept Math, Cambridge, MA 02142 USA

[5] Imperial Coll London, Inst Mol Sci & Engn, South Kensington Campus, London SW7 2AZ, England

来源：

JOURNAL OF CHEMICAL PHYSICS | 2022年 / 157卷 / 09期

基金：

英国工程与自然科学研究理事会; 美国国家科学基金会;

关键词：

WATER-IN-SALT; THERMOREVERSIBLE GELATION; SOLVENT-FREE; ELECTROLYTES; CAPACITANCE; TRANSPORT; SURFACE; CHARGE; HETEROGENEITY; ORGANIZATION;

D O I：

10.1063/5.0097055

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

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. (c) 2022 Author(s).

引用

页数：16

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