Mesoscale Inhomogeneities in Aqueous Solutions of 3-Methylpyridine and Tertiary Butyl Alcohol

Subramanian, Deepa; Иванов, Д. А.; Yudin, I. K.; Анисимов, М. А.; Sengers, J. V.

doi:10.1021/je101125e

Cited by 62 publications

(113 citation statements)

References 69 publications

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“…Possible evidence of inhomogeneities was found by LLS studies of aqueous solutions of 3-methylpyridine and tertiary butyl alcohol [79]. The observed inhomogeneities were attributed to near-spherical Brownian aggregates of sizes from a hundred to a few hundred nm.…”

Section: Large-scale Inhomogeneities In Aqueous Systems And/or Exclusmentioning

confidence: 94%

“…The features of EZ water, in our opinion, also play an important role in the development of the thixotropic phenomenon that could be further confirmed by large-scale inhomogeneities found in aqueous systems. Literature indicating large scale inhomogeneities in aqueous solutions is accumulating, with emphasis on static and dynamic laser light scattering (LLS) measurements [69][70][71][72][73][74][75][76][77][78][79][80]. A wide variety of other experimental techniques may confirm that in aqueous under-saturated strong electrolyte solutions, the ions are not homogeneously distributed [63,[81][82][83][84][85][86].…”

Section: Large-scale Inhomogeneities In Aqueous Systems And/or Exclusmentioning

confidence: 99%

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Possible Further Evidence for the Thixotropic Phenomenon of Water

Verdel

Bukovec

2014

Entropy

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Abstract:In this work we review the literature for possible confirmation of a phenomenon that was proposed to develop when water is left to stand for some time undisturbed in closed vessels. The phenomenon has been termed thixotropy of water due to the weak gel-like behaviour which may develop spontaneously over time where ions and contact with hydrophilic surfaces seem to play important roles. Thixotropy is a property of certain gels and liquids that under normal conditions are highly viscous, whereas during mechanical processing their viscosity diminishes. We found experiments indicating water's self-organizing properties, long-lived inhomogeneities and time-dependent changes in the spectral parameters of aqueous systems. The large-scale inhomogeneities in aqueous solutions seem to occur in a vast number of systems. Long-term spectral changes of aqueous systems were observed even though the source of radiation was switched off or removed. And water was considered to be an active excitable medium in which appropriate conditions for self-organization can be established. In short, the thixotropic phenomenon of water is further indicated by different experimental techniques and may be triggered by large-scale ordering of water in the vicinity of nucleating solutes and hydrophilic surfaces.

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Section: Large-scale Inhomogeneities In Aqueous Systems And/or Exclusmentioning

confidence: 94%

Section: Large-scale Inhomogeneities In Aqueous Systems And/or Exclusmentioning

confidence: 99%

Possible Further Evidence for the Thixotropic Phenomenon of Water

Verdel

Bukovec

2014

Entropy

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“…[28,29,31,32]. In Moscow, the measurements were performed at the scattering angles of 20, 30 and 90 .…”

Section: Light Scatteringmentioning

confidence: 99%

“…It has been shown that such inhomogeneities occur in aqueous solutions of nonionic hydrotropes when the solution contains a third, more hydrophobic, component [12,13,[28][29][30][31][32]. Remarkably, these inhomogeneities (emerging in water-rich ternary systems) are only pronounced in the hydrotrope concentration range where molecular clustering and thermodynamic anomalies are observed in the original binary hydrotrope-water solutions.…”

Section: Introductionmentioning

confidence: 99%

Mesoscale solubilization and critical phenomena in binary and quasi-binary solutions of hydrotropes

Robertson

Phan

Macaluso

et al. 2016

Fluid Phase Equilibria

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A B S T R A C THydrotropes are substances consisting of amphiphilic molecules that are too small to self-assemble in equilibrium structures in aqueous solutions, but can form dynamic molecular clusters H-bonded with water molecules. Some hydrotropes, such as low-molecular-weight alcohols and amines, can solubilize hydrophobic compounds in aqueous solutions at a mesoscopic scale ($100 nm) with formation of longlived mesoscale droplets. In this work, we report on the studies of near-critical and phase behavior of binary (2,6-lutidine-H 2 O) and quasibinary (2,6-lutidine-H 2 O/D 2 O and tert-butanol/2-butanol-H 2 O) solutions in the presence of a solubilized hydrophobic impurity (cyclohexane). In additional to visual observation of fluid-phase equilibria, two experimental techniques were used: light scattering and smallangle neutron scattering. It was found that the increase of the tert-butanol/2-butanol ratio affects the liquid-liquid equilibria in the quasi-binary system at ambient pressure in the same way as the increase of pressure modifies the phase behavior of binary 2-butanol-H 2 O solutions. The correlation length of critical fluctuations near the liquid-liquid separation and the size of mesoscale droplets of solubilized cyclohexane were obtained by dynamic light scattering and by small-angle neutron scattering. It is shown that the effect of the presence of small amounts of cyclohexane on the near-critical phase behavior is twofold: (1) the transition temperature changes toward increasing the two-phase domain; (2) longlived mesoscopic inhomogeneities emerge in the macroscopically homogeneous domain. These homogeneities remain unchanged upon approach to the critical point of macroscopic phase separation and do not alter the universal nature of criticality. However, a larger amount of cyclohexane generates additional liquid-liquid phase separation at lower temperatures.

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“…Such long living mesoscopic structures shown in Fig. 7 become an interesting topic of research in its own right [57,58,98].…”

Section: Experiments Determining the Nature Of The Critical Pointmentioning

confidence: 99%

A Short History of Phase Transitions in Ionic Fluids

Schröer

2012

Contrib. Plasma Phys.

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The paper reviews the development of theory and experiments concerning the nature of the critical point in ionic fluids. Because of the long-range nature of the Coulomb interactions the possibility of mean-field critical behaviour was discussed as a possibility. Although some experiments supported mean-field criticality, simulations on the model fluid of charged hard spheres and later experiments on ionic solutions have shown that phase transition of ionic systems belong to the Ising universality class like phase transitions in non-ionic fluids. Experiments concerning the crossover from Ising to mean field-behaviour are discussed as well as systematic differences between the phase behaviour predicted for the model fluid of charged hard spheres and that observed in ionic solutions.

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Mesoscale Inhomogeneities in Aqueous Solutions of 3-Methylpyridine and Tertiary Butyl Alcohol

Cited by 62 publications

References 69 publications

Possible Further Evidence for the Thixotropic Phenomenon of Water

Possible Further Evidence for the Thixotropic Phenomenon of Water

Mesoscale solubilization and critical phenomena in binary and quasi-binary solutions of hydrotropes

A Short History of Phase Transitions in Ionic Fluids

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