Direct observation of time-temperature-transformation curves for crystallization of ice from solutions by a homogeneous mechanism

MacFarlane, Douglas R.; Kadiyala, R. K.; Angell, C. Austen

doi:10.1021/j100230a002

Cited by 28 publications

(12 citation statements)

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“…A separate factor is the growth rate of nuclei, which always increases with increasing temperatures except near the liquidus (25). The maximum crvstallization rate is found at temperatures 'somewhat above the temperature of maximum nucleation rate and is easily determined by isothermal calorimetry studies (32).…”

Section: Beating the Crystallization Trap T O Workersmentioning

confidence: 99%

Formation of Glasses from Liquids and Biopolymers

Angell

1995

Science

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Glasses can be formed by many routes. In some cases, distinct polyamorphic forms are found. The normal mode of glass formation is cooling of a viscous liquid. Liquid behavior during cooling is classified between "strong" and "fragile," and the three canonical characteristics of relaxing liquids are correlated through the fragility. Strong liquids become fragile liquids on compression. In some cases, such conversions occur during cooling by a weak first-order transition. This behavior can be related to the polymorphism in a glass state through a recent simple modification of the van der Waals model for tetrahedrally bonded liquids. The sudden loss of some liquid degrees of freedom through such first-order transitions is suggestive of the polyamorphic transition between native and denatured hydrated proteins, which can be interpreted as single-chain glass-forming polymers plasticized by water and cross-linked by hydrogen bonds. The onset of a sharp change in ddT( is the Debye-Waller factor and T is temperature) in proteins, which is controversially indentified with the glass transition in liquids, is shown to be general for glass formers and observable in computer simulations of strong and fragile ionic liquids, where it proves to be close to the experimental glass transition temperature. The latter may originate in strong anharmonicity in modes ("bosons"), which permits the system to access multiple minima of its configuration space. These modes, the Kauzmann temperature T(K), and the fragility of the liquid, may thus be connected.

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Section: Beating the Crystallization Trap T O Workersmentioning

confidence: 99%

Formation of Glasses from Liquids and Biopolymers

Angell

1995

Science

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4,437

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“…Study of vitrified aqueous solutions of LiCl has suggested the existence of liquidliquid immiscibility and polyamorphism about half a century ago [7,8]. In particular, Angell and coworkers performed detailed studies of the behaviour of LiCl aqueous solutions, including the study of the glass transition tem-perature (T g ) as a function of composition and pressure, homogeneous and heterogenous nucleation, and ice crystallization [8][9][10][11]. Also Kanno inferred the existence of liquid-liquid immiscibility by studying LiCl aqueous solutions at high pressures [12].…”

Section: Introductionmentioning

confidence: 99%

Pressure-induced transformations in LiCl–H₂O at 77 K

Ruiz

Bove

Corti

et al. 2014

Phys. Chem. Chem. Phys.

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A systematic study of the properties of high-density amorphous ice (HDA) in the presence of increasing amounts of salt is missing, especially because it is challenging to avoid ice crystallization upon cooling the pressurized liquid. In order to be able to study HDA also in the presence of small amounts of salt, we have investigated the transformation behaviour of quenched aqueous LiCl solutions (mole fraction x < 0.25) upon pressurization in a piston-cylinder setup at 77 K. The sample properties were characterized by in situ dilatometry under high pressure conditions and after recovery by ex situ powder X-ray diffraction (XRD) and differential scanning calorimetry (DSC) at ambient pressure. Two regimes can be identified, with a rather sharp switch at about x = 0.12. At x < 0.12 the samples show the phenomenology also known for pure water samples. They are composed mainly of hexagonal ice (Ih) and experience pressure-induced amorphization to HDA at P > 1 GPa. The observed densification is consistent with the idea that a freeze concentrated LiCl solution of x = 0.14 (R = 6) segregates, which transforms to the glassy state upon cooling, and that the densification is only due to the Ih → HDA transition. Also the XRD patterns and DSC scans are almost unaffected by the presence of the segregated glassy LiCl solution. Upon heating at ambient pressure HDA experiences the polyamorphic transition to low-density amorphous ice (LDA) at ∼120 K, even at x ∼ 0.10. Based on the latent heat evolved in the transition we suggest that almost all water in the sample transforms to an LDA-like state, even the water in the vicinity of the ions. The glassy LiCl solution acts as a spectator that does not shift the transformation temperature significantly and experiences a glass-to-liquid transition at ∼140 K prior to the crystallization to cubic ice. By contrast, at x > 0.12 the phenomenology completely changes and is now dominated by the salt. Hexagonal ice no longer forms upon quenching the LiCl solution, but instead LDA forms. A broad pressure-induced transformation at >0.6 GPa can be attributed to the densification of LDA, the glassy LiCl solution and/or glassy hydrates.

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“…It is expected that the homogeneous nucleation takes place in this Tc range (Clausse et al, 1983;MacFarlane et al, 1983). The different Tc dependence of Tm, is due to the difference in crystal growth.…”

Section: Resultsmentioning

confidence: 98%

Crystallization of Water in the Xanthan-Water System

Yoshida

Hatakeyama

Hatakeyama³

1993

Journal of Intelligent Material Systems and Structures

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Isothermal crystallization of water in polysaccharide hydrogels was measured by differential scanning calorimetry (DSC). The melting temperature ( Tm 1 ) of ice depended on the crystallization temperature (Tc) for freezing bound water, which was restrained by hydrogels. However, the Tm 1 of free water and pure water were constant regardless of Tc. These facts suggested that freezing bound water formed metastable ice. The nucleation rates of pure water, free water and freezing bound water were almost the same in the temperature range examined. Pure water showed the highest rate of crystal growth. The crystal growth rate decreased in the following order: pure water > free water > freezing bound water. The average surface free energy of ice was estimated from the rate of crystal growth. The estimated values of surface free energy of ice from freezing bound water were lower than that of ice from pure water. The results suggested that not only water molecules, but also polysaccharide molecules and ions existed on the surface of ice formed in the hydrogels.

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Direct observation of time-temperature-transformation curves for crystallization of ice from solutions by a homogeneous mechanism

Cited by 28 publications

References 0 publications

Formation of Glasses from Liquids and Biopolymers

Formation of Glasses from Liquids and Biopolymers

Pressure-induced transformations in LiCl–H₂O at 77 K

Crystallization of Water in the Xanthan-Water System

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Direct observation of time-temperature-transformation curves for crystallization of ice from solutions by a homogeneous mechanism

Cited by 28 publications

References 0 publications

Formation of Glasses from Liquids and Biopolymers

Formation of Glasses from Liquids and Biopolymers

Pressure-induced transformations in LiCl–H2O at 77 K

Crystallization of Water in the Xanthan-Water System

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Pressure-induced transformations in LiCl–H₂O at 77 K