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Toward an Understanding of the Mechanisms behind the Formation of Liquid-liquid Systems formed by Two Ionic Liquids.

ABSTRACT: Biphasic systems composed of aprotic ionic liquids (ILs) allow the development of new separation processes constituted only by nonvolatile solvents. Six pairs of cholinium- and phosphonium-based ILs were found to be able to form biphasic systems, and the respective liquid-liquid phase diagrams were determined. Although IL anions do not seem to control the phase separation phenomenon, they play an important role in defining the size of the biphasic region. A linear dependence of the ILs mutual solubilities with the IL anions volume was found, supporting the relevance of the entropy of mixing. With the exception of the system formed by ILs with a common anion, the remaining liquid-liquid systems display a significant ion exchange extent between the phases, which inversely depends on the ILs cohesive energy. It is finally shown that four-phase systems with a remarkable performance in the separation of mixtures of dyes can be prepared.

SUBMITTER: Neves CMSS

PROVIDER: S-EPMC6157719 | biostudies-literature | 2017 Jul

REPOSITORIES: biostudies-literature

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Toward an Understanding of the Mechanisms behind the Formation of Liquid-liquid Systems formed by Two Ionic Liquids.

Neves Catarina M S S CMSS Silva Artur M S AMS Fernandes Ana M AM Coutinho João A P JAP Freire Mara G MG

The journal of physical chemistry letters 20170619 13

Biphasic systems composed of aprotic ionic liquids (ILs) allow the development of new separation processes constituted only by nonvolatile solvents. Six pairs of cholinium- and phosphonium-based ILs were found to be able to form biphasic systems, and the respective liquid-liquid phase diagrams were determined. Although IL anions do not seem to control the phase separation phenomenon, they play an important role in defining the size of the biphasic region. A linear dependence of the ILs mutual so ...[more]

PMID: 28609628

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Project description:By mixing ionic liquids (ILs), it is possible to fine-tune their bulk and interfacial structure. This alters their physical properties and solvation behavior and is a simple way to prepare a collection of ILs whose properties can be tuned to optimize a specific application. In this study, mixtures of perfluorinated and alkylated ILs have been prepared, and links between composition, properties, and nanostructure have been investigated. These different classes of ILs vary substantially in the flexibility and polarizability of their chains. Thus, a range of useful structural and physical property variations are accessible through mixing that will expand the library of IL mixtures available in an area that to this point has received relatively little attention. In the experiments presented herein, the physical properties and bulk structure of mixtures of 1-methyl-3-octylimidazolium bis(trifluoromethylsulfonyl)imide [C8MIM][Tf2N] and 1-(1H,1H,2H,2H-perfluorooctyl)-3-methylimidazolium bis(trifluoromethylsulfonyl)imide [C8MIM-F13][Tf2N] have been prepared. The bulk liquid structure was investigated using a combination of small-angle X-ray and neutron scattering (SAXS and SANS, respectively) experiments in combination with atomistic molecular dynamics simulations and the measurement of density and viscosity. We observed that the addition of [C8MIM-F13][Tf2N] to [C8MIM][Tf2N] causes changes in the nanostructure of the IL mixtures that are dependent on composition so that variation in the characteristic short-range correlations is observed as a function of composition. Thus, while the length scales associated with the apolar regions (polar non-polar peak─PNPP) increase with the proportion of [C8MIM-F13][Tf2N] in the mixtures, perhaps surprisingly given the greater volume of the fluorocarbon chains, the length scale of the charge-ordering peak decreases. Interestingly, consideration of the contact peak shows that its origins are both in the direct anion···cation contact length scale and the nature (and hence volume) of the chains appended to the imidazolium cation.

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Toward an Understanding of the Mechanisms behind the Formation of Liquid-liquid Systems formed by Two Ionic Liquids.

Publications

Toward an Understanding of the Mechanisms behind the Formation of Liquid-liquid Systems formed by Two Ionic Liquids.

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