Correlated Ion Transport and the Gel Phase in Room Temperature Ionic Liquids

Here we present a theory of ion aggregation and gelation of room temperature ionic liquids (RTILs). Based on it, we investigate the effect of ion aggregation on correlated ion transportionic conductivity and transference numbersobtaining closed-form expressions for these quantities. The theory dep...

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Published inThe journal of physical chemistry. B Vol. 125; no. 10; pp. 2677 - 2689
Main Authors McEldrew, Michael, Goodwin, Zachary A. H, Zhao, Hongbo, Bazant, Martin Z, Kornyshev, Alexei A
Format Journal Article
LanguageEnglish
Published United States American Chemical Society 18.03.2021
Subjects
B: Liquids; Chemical and Dynamical Processes in Solution
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Abstract Here we present a theory of ion aggregation and gelation of room temperature ionic liquids (RTILs). Based on it, we investigate the effect of ion aggregation on correlated ion transportionic conductivity and transference numbersobtaining closed-form expressions for these quantities. The theory depends on the maximum number of associations a cation and anion can form and the strength of their association. To validate the presented theory, we perform molecular dynamics simulations on several RTILs and a range of temperatures for one RTIL. The simulations indicate the formation of large clusters, even percolating through the system under certain circumstances, thus forming a gel, with the theory accurately describing the obtained cluster distributions in all cases. However, based on the strength and lifetime of associations in the simulated RTILs, we expect free ions to dominate ionic conductivity despite the presence of clusters, and we do not expect the percolating cluster to trigger structural arrest in the RTIL.
AbstractList Here we present a theory of ion aggregation and gelation of room temperature ionic liquids (RTILs). Based on it, we investigate the effect of ion aggregation on correlated ion transportionic conductivity and transference numbersobtaining closed-form expressions for these quantities. The theory depends on the maximum number of associations a cation and anion can form and the strength of their association. To validate the presented theory, we perform molecular dynamics simulations on several RTILs and a range of temperatures for one RTIL. The simulations indicate the formation of large clusters, even percolating through the system under certain circumstances, thus forming a gel, with the theory accurately describing the obtained cluster distributions in all cases. However, based on the strength and lifetime of associations in the simulated RTILs, we expect free ions to dominate ionic conductivity despite the presence of clusters, and we do not expect the percolating cluster to trigger structural arrest in the RTIL.
Here we present a theory of ion aggregation and gelation of room temperature ionic liquids (RTILs). Based on it, we investigate the effect of ion aggregation on correlated ion transport-ionic conductivity and transference numbers-obtaining closed-form expressions for these quantities. The theory depends on the maximum number of associations a cation and anion can form and the strength of their association. To validate the presented theory, we perform molecular dynamics simulations on several RTILs and a range of temperatures for one RTIL. The simulations indicate the formation of large clusters, even percolating through the system under certain circumstances, thus forming a gel, with the theory accurately describing the obtained cluster distributions in all cases. However, based on the strength and lifetime of associations in the simulated RTILs, we expect free ions to dominate ionic conductivity despite the presence of clusters, and we do not expect the percolating cluster to trigger structural arrest in the RTIL.
Author McEldrew, Michael
Kornyshev, Alexei A
Zhao, Hongbo
Bazant, Martin Z
Goodwin, Zachary A. H
AuthorAffiliation Department of Chemistry
Thomas Young Centre for Theory and Simulation of Materials
Department of Chemical Engineering
Institute of Molecular Science and Engineering
Department of Mathematics
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  givenname: Zachary A. H
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  surname: Goodwin
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  givenname: Hongbo
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BackLink https://www.ncbi.nlm.nih.gov/pubmed/33689352$$D View this record in MEDLINE/PubMed
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Snippet Here we present a theory of ion aggregation and gelation of room temperature ionic liquids (RTILs). Based on it, we investigate the effect of ion aggregation...
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SubjectTerms B: Liquids; Chemical and Dynamical Processes in Solution
Title Correlated Ion Transport and the Gel Phase in Room Temperature Ionic Liquids
URI http://dx.doi.org/10.1021/acs.jpcb.0c09050
https://www.ncbi.nlm.nih.gov/pubmed/33689352
https://search.proquest.com/docview/2500385967
Volume 125
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