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Utilizing Infrared Spectroscopy to Analyze the Interfacial Structures of Ionic Liquids/Al₂O₃ and Ionic Liquids/Mica Mixtures under High Pressures.

ABSTRACT: The interfacial interactions between ionic liquids (1,3-dimethylimidazolium methyl sulfate and 1-ethyl-3-methylimidazolium trifluoromethanesulfonate) and solid surfaces (mesoporous aluminum oxide and mica) have been studied by infrared spectroscopy at high pressures (up to 2.5 GPa). Under ambient pressure, the spectroscopic features of pure ionic liquids and mixtures of ionic liquids/solid particles (Al₂O₃ and mica) are similar. As the pressure is increased, the cooperative effect in the local structure of pure 1,3-dimethylimidazolium methyl sulfate becomes significantly enhanced as the imidazolium C⁻H absorptions of the ionic liquid are red-shifted. However, this pressure-enhanced effect is reduced by adding the solid particles (Al₂O₃ and mica) to 1,3-dimethylimidazolium methyl sulfate. Although high-pressure IR can detect the interactions between 1,3-dimethylimidazolium methyl sulfate and particle surfaces, the difference in the interfacial interactions in the mixtures of Al₂O₃ and mica is not clear. By changing the type of ionic liquid to 1-ethyl-3-methylimidazolium trifluoromethanesulfonate, the interfacial interactions become more sensitive to the type of solid surfaces. The mica particles in the mixture perturb the local structure of 1-ethyl-3-methylimidazolium trifluoromethanesulfonate under high pressures, forcing 1-ethyl-3-methylimidazolium trifluoromethanesulfonate to form into an isolated structure. For Al₂O₃, 1-ethyl-3-methylimidazolium trifluoromethanesulfonate tends to form an associated structure under high pressures.

SUBMITTER: Chang YH

PROVIDER: S-EPMC6473959 | biostudies-literature |

REPOSITORIES: biostudies-literature

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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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Utilizing Infrared Spectroscopy to Analyze the Interfacial Structures of Ionic Liquids/Al₂O₃ and Ionic Liquids/Mica Mixtures under High Pressures.

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