Specific features of crystallization of supersaturated solution in femtoliter-volume systems

Titaeva, E. K.; Fedoseev, V. B.

doi:10.1134/s1063774514030195

Cited by 10 publications

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“…In similar experiments with solutions of individual KCl or NaCl salts in droplets of the same dimension, one or two single crystals with regular faceting are usu ally formed [9]. The evaporation of the solution of the mixture of KCl and NaCl is accompanied by the for mation of a polycrystalline structure.…”

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Solution-crystal-solution oscillatory phase transitions in the KCl-NaCl-H2O system

Fedoseev

Maksimov

2015

Jetp Lett.

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390Microscopic studies of size effects at phase transi tions revealed unusual kinetic features. Under almost stationary conditions, in an ensemble of droplets of an aqueous solution of a mixture of nonvolatile com pounds, multiple repeated processes of evaporationcondensation of droplets of the solution with the for mation of a crystal and subsequent condensation of water on the crystal, which completely recovered the dimensions of droplets, were observed. Solutioncrystal oscillations occurred with a frequency of sev eral oscillations per minute. They were not interrupted until stationary conditions were maintained.The most well known observations of an oscilla tory regime at a phase transition are Liesegang rings described at the end of the 19th century [1]. The first theoretical interpretation of this phenomenon was proposed by Ostwald. The formation of Liesegang ring type structures is usually irreversible in both time and space. A periodic phase transition was described for a lattice model [2]. However, this two dimensional mathematical model is inapplicable to the description of a heterogeneous three component system and can not describe mass transfer between three phases.Pulsations of the temperature and pressure at the evaporation of sessile droplets were described in [3]. The effect appeared in multicomponent, unlimitedly mutual soluble mixtures of volatile components (water-ethanol-methanol). A theoretical interpreta tion proposed by the authors of that work is based on the description of a diffusive water flux through the interface between phases at a given temperature drop with the imposition of a pulsation. The chemical ¶ See the supplemental materials to this article at the website www.jetpletters.ac.ru potentials of the components of the imperfect solution are determined by the concentrations of all sub stances. This relation (equations of state) usually has a quite complex form. Diffuse fluxes generated by the difference between chemical potentials in a real solu tion also depend on the concentrations of all compo nents. This possibly explains why oscillations were observed experimentally only in multicomponent sys tems.The oscillatory regime of nucleation of droplets was observed in counterpropagating fluxes of vapors and falling droplets [4]. In this case, oscillations occur not with individual droplets, but at the condensation of supersaturated vapor.Oscillations described in [3,4] have a common nature with phenomena observed in our experiments. Oscillations occur owing to diffusive fluxes at the interface between phases, where one of the phases is far from the state of an ideal solution.Phase transitions discussed in this work occur under almost stationary conditions and are accompa nied by reversible condensation: evaporation of the liquid phase with simultaneous condensation-solu tion of the crystal phase. The mass of the system changes significantly at multiple transitions from the "crystal" state to the "crystal + solution" state and back in observed oscillations. As far as we know, such a ...

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“…The method used in this work is based on the microscopic observation of an ensemble of evaporat ing droplets of a solution of nonvolatile compounds and was described in [8,9]. The ensemble of droplets of a diluted solution was deposited by an atomizer on the slide of an MBS 1 microscope.…”

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Solution-crystal-solution oscillatory phase transitions in the KCl-NaCl-H2O system

Fedoseev

Maksimov

2015

Jetp Lett.

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“…Некоторые кинетические особенности фазовых превращений в многокомпонентных дисперсных системах (ансамбле капель раствора) впервые описаны в [8][9][10][11]. Одной из них является неоствальдовское поведение (НП), при котором испарение мелких капель и кристаллизация в них происходят медленнее, чем в крупных.…”

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“…Одной из них является неоствальдовское поведение (НП), при котором испарение мелких капель и кристаллизация в них происходят медленнее, чем в крупных. В [8,9] описаны наблюдения НП в реальном времени для ансамблей сидячих капель водных растворов неорганических солей. В общем виде интерпретация НП предложена в [8], более простое обоснование можно связать с разнонаправленным действием процессов, описываемых уравнением Кельвина−Оствальда и законом Рауля [11].…”

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“…Неоспоримой демонстрацией НП являются визуальные микроскопические наблюдения в реальном времени [8,9]. Эти простые и доступные эксперименты хорошо воспроизводятся для водных растворов ряда неорганических солей (NaCl, KCl, NaNO 3 , NH 4 Cl и др.…”

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Неоствальдовское Поведение Дисперсных Систем В Процессах Испарения И Кристаллизации Капель Водно-Органических Растворов

Федосеева¹,

Федосеев²

2020

Журнал Технической Физики

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In this paper, experiments with water-based solutions of some organic compounds, which demonstrate non-Ostwald behavior have been described. Small-volume droplets demonstrate higher stability during evaporation and crystallization in comparison with larger ones, such an effect has been previously described only for water-based solutions of inorganic salts. It has been shown that non-Ostwald behavior has the same thermodynamic nature with Ostwald ripening and could occur in dispersed systems of a complicated chemical composition. Peculiar realization of such phenomena driven by surface activity of organic compounds in water solutions has also been described. The studied regularities could be used to obtain solutions of organic and bioorganic substances with concentrations significantly higher than their solubility limits under normal conditions as well as to reproduce narrow size distributions of droplets in various spray technologies.

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Formation of BI- and Polymodal Distributions and the Non-Ostwald Behavior of Disperse Systems

Fedoseev

Fedoseeva

2019

J Eng Phys Thermophy

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Specific features of crystallization of supersaturated solution in femtoliter-volume systems

Cited by 10 publications

References 16 publications

Solution-crystal-solution oscillatory phase transitions in the KCl-NaCl-H2O system

Solution-crystal-solution oscillatory phase transitions in the KCl-NaCl-H2O system

Неоствальдовское Поведение Дисперсных Систем В Процессах Испарения И Кристаллизации Капель Водно-Органических Растворов

Formation of BI- and Polymodal Distributions and the Non-Ostwald Behavior of Disperse Systems

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