Nanophase separation in aqueous dilutions of a ternary DES as revealed by Brillouin and NMR spectroscopy

Posada, E.; Roldán-Ruiz, María J.; Riobóo, R. J. Jiménez; Gutiérrez, Marı́a C.; Ferrer, M. Luisa; Monte, Francisco del

doi:10.1016/j.molliq.2018.11.139

Cited by 38 publications

(37 citation statements)

References 68 publications

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“…From a thermodynamic or structural point of view, it may be considered that the unfrozen water molecules retained in the DES system during ice formation are involved in the formation of stable structures. Recent Brillouin studies have indicated the existence of a crossover in the sound propagation velocity in different DES for an aqueous dilution around W=30% [17,18]. Along with NMR data, this result has been interpreted as the transitioning of the liquid structure from a H 2 O-based to a DES-based H-bonded network.…”

Section: J O U R N a L P R E -P R O O F 20mentioning

confidence: 86%

“…The integrity of DES could be destroyed in biphasic aqueous systems, while its local arrangement could be preserved in single-phase aqueous DES mixtures up to a moderate degree of hydration [1,11]. The physical properties of water-ionic liquids and water-DES mixtures, including excess properties, viscosity, acoustic, structural and optical properties have been studied around ambient temperature and above [1,[12][13][14][15][16][17][18][19].…”

Section: J O U R N a L P R E -P R O O Fmentioning

confidence: 99%

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Phase behavior of aqueous solutions of ethaline deep eutectic solvent

Jani

Sohier

Morineau

2020

Journal of Molecular Liquids

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We have established a detailed phase diagram of a prototypical DES as a function of the hydration level. Two distinct thermal phase behaviors are observed depending on the water content with respect to a cross-over composition W g ' = 30%. For W < W g ', the formation of ice is not observed under the experimental conditions used in this study, and the solution falls in the category of glassforming systems. Fully vitreous states could also be obtained between 30% and 50%, but they are metastable with respect to water crystallization. For W > W g ', ice crystallization occurs but the residual DES solution remains amorphous (liquid or glassy). In the latter case, whatever the initial water fraction, this transformation finally ends at the fixed composition W g ' corresponding to 6 to 10 water molecules per choline ion for the two studied DESs. We infer that the residual liquid water molecules forming this maximally freeze-concentrated solution are strongly interacting with DES molecular units. This situation is also known as the "water-in-DES" case. Conversely, ice crystallization concerns free water molecules, provided that W > W g ', also known as the "DES-in-water" case. This entire phase behavior is explained in the context of maximally freeze-concentrated solutions and attributed to the concomitant effects of ice freezing depression, glassforming ability of weakly hydrated DES Journal Pre-proof J o u r n a l P r e-p r o o f 2 (W < W g ') and water structure distortion. This study also highlights the potential of DESs for their uses in freeze-drying processes and biopreservative applications.

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Section: J O U R N a L P R E -P R O O F 20mentioning

confidence: 86%

Section: J O U R N a L P R E -P R O O Fmentioning

confidence: 99%

Phase behavior of aqueous solutions of ethaline deep eutectic solvent

Jani

Sohier

Morineau

2020

Journal of Molecular Liquids

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“…Distilled H2O, fresh Reagent 1 (R1) and R1 measurement after heart and brain clearing. 90A scattering geometry and backscattering geometry were used simultaneously in order to asses hypersonic sound velocity and refractive index [27]. For comparison, the refractive index was also measured with a standard Abbe refractometer (nA).…”

Section: Cubic Clearing In Brain and Cardiac Mouse Tissuementioning

confidence: 99%

Impact of optical tissue clearing on the Brillouin signal from biological tissue samples

Riobóo

Desco

Gómez-Gaviro

2019

Biomed. Opt. Express

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Brillouin spectroscopy is a well-established technology in condensed matter physics to characterize the mechanical properties of inert materials, and it has been extended very recently to the study of biological samples. Transparency is beneficial for samples to be properly analyzed by Brillouin spectroscopy. Here, we explored the efficacy of optical tissue clearing techniques to improve the acquisition of Brillouin spectra from biological tissues in order to analyze their biomechanical properties. We describe the first application of Brillouin scattering to optically cleared biological tissues with CUBIC protocol. We conclude that, within the range of error, tissue clearing does not modify the mechanical properties of the studied biological tissues.

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“…For practical reasons, aqueous solutions of DESs have been formulated and their physical properties, including excess properties, viscosity, acoustic, structural and optical properties have been studied thoroughly. [9][10][11][12][13][14][15][16][17][18][19][20][21] These works have also raised the question of the resilience of the specific local arrangement of DES during dilution with water and its evolution towards an aqueous solution of its constituents. 9-11, 19, 22 The structure of DESs has attracted a lot of interest during the last four years.…”

Section: Introductionmentioning

confidence: 99%

Do Deep Eutectic Solvents Form Uniform Mixtures Beyond Molecular Microheterogeneities?

et al. 2020

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We have performed small angle neutron scattering (SANS) in a momentum transfer range (0.05 < Q < 0.5 Å -1 ) to study long range order and concentration fluctuations in deep eutectic solvents (DESs) and their aqueous solutions. Ethaline (choline chloride:ethylene glycol), glycerol:lactic acid, and menthol:decanoic acid mixtures were selected to illustrate respectively the case of ionic, nonionic and hydrophobic mixtures. Different carefully designed isotopic labelling was used to emphasize selectively the spatial correlations between the different solvent components. For ethaline DESs and their aqueous solutions, a weak low-Q peak observed only for certain compositions and some partial structure factors revealed the mesoscopic segregation of ethylene glycol molecules that do not participate to the solvation of ionic units, either because they are in excess with respect the eutectic stoichiometry (1:4 neat ethaline) or substituted by water 2 (4w-ethaline and higher aqueous dilutions). For the nonionic hydrophilic solutions, such a mesoscopic segregation was not observed. This indicates that the better balanced interactions between the three nonionic H-bonded components (water, lactic acid, and glycerol) favor homogeneous mixing. For the hydrophobic DESs, we observed an excess of coherent scattering intensity centered at Q = 0, which could be reproduced by a model of non-interacting spherical domains. Local concentration fluctuations are not excluded either. However, unlike liquid mixtures with a tendency to demix, we have found no evidence of expansion of domains with different compositions to a large scale.

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Nanophase separation in aqueous dilutions of a ternary DES as revealed by Brillouin and NMR spectroscopy

Cited by 38 publications

References 68 publications

Phase behavior of aqueous solutions of ethaline deep eutectic solvent

Phase behavior of aqueous solutions of ethaline deep eutectic solvent

Impact of optical tissue clearing on the Brillouin signal from biological tissue samples

Do Deep Eutectic Solvents Form Uniform Mixtures Beyond Molecular Microheterogeneities?

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