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A special issue of Crystals (ISSN 2073-4352). This special issue belongs to the section "Inorganic Crystalline Materials".

Deadline for manuscript submissions: closed (31 March 2019) | Viewed by 50143

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Prof. Dr. Yoshinori Furukawa

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Guest Editor

Institute of Low Temperature Science, Hokkaido University, Sapporo 060-0808, Japan
Interests: biophysics; ice physics; crystal growth

Special Issue Information

Dear Colleagues,

Ice crystals are the most ubiquitous material in the cryosphere environment of the Earth, in the planetary system, and also in our daily lives. In recent years, ice crystals have increased in importance as one of the key materials for finding solutions to settle various environmental concerns at a global scale. Furthermore, ice crystals are also expected as one of the unique materials which are extremely useful to various applications, for example, the food sciences, medical sciences, and other various fields. Dealing with these interesting subjects, research on ice crystals has been more actively pursued in recent years.

The current Special issue of Crystals provides a unique forum for the discussion and presentation of recent advances in study of ice crystals. Since research on ice crystals is included in many different fields, communications and discussions among researchers are not sufficient, nor are they smooth. Publications related to ice crystals are also distributed in various journals, such as those dealing with physics, chemistry, biology, geoscience, planetary science, crystal growth, and others. Consequently, this Special issue will provide a platform for discussions among the researchers working in different fields.

The topics summarized under the keywords should be considered only as examples. The volume is open for any advanced topics related to ice crystals. We expect to be combined many papers which discuss the ice crystals in the various research fields.

Prof. Dr. Yoshinori Furukawa
Guest Editor

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Keywords

Crystal structures
Phase transitions
Surfaces and interfaces
Defects
Crystal growth
Clathrate hydrates
Chemical aspects
Biological aspects
Glaciological aspects
Planetary aspects
Others

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Published Papers (12 papers)

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Editorial

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2 pages, 144 KiB

Open AccessEditorial

Ice Crystals

by Yoshinori Furukawa

Crystals 2019, 9(10), 540; https://doi.org/10.3390/cryst9100540 - 19 Oct 2019

Viewed by 2664

Abstract

The special issue on “Ice Crystals” includes seven contributed papers, which give the wide varieties of topics related to ice crystals. They focus on the interface structure of ice, the physical properties of hydrate crystals and the freezing properties of water controlled by antifreeze proteins. The present issue can be considered as a status report reviewing the research that has been made recently on ice crystals. These papers provide research information about the recent development of ice crystal research to readers. Full article

(This article belongs to the Special Issue Ice Crystals)

Research

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9 pages, 2943 KiB

Open AccessArticle

Numerical Simulation of Ice Fractures Process of the Yellow River Based on Disk Specimen

by Juan Wang, Jiao Zhou, Yu Deng, Goncharov Vadim and Peng Zhang

Crystals 2020, 10(7), 598; https://doi.org/10.3390/cryst10070598 - 10 Jul 2020

Cited by 9 | Viewed by 2635

Abstract

To study the influence of the changes in crystals on a micro scale as well as their effect on the macro mechanical properties of river ice and to mitigate the limitation of the objective conditions in a physical examination of river ice, it is necessary to analyze the fracture process of river ice using a micro numerical calculation method. Thus, a numerical model was established to simulate the cracking process of river ice based on disk specimen. Upon comparison with the physical experiment, the results of the numerical model show agreement with the fracture toughness and cracking process. Based on the numerical model, the obtained material parameters of Yellow River ice laid a foundation for the study of the cracking process of river ice on a macro-, meso-, and multiscale. Full article

(This article belongs to the Special Issue Ice Crystals)

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15 pages, 1820 KiB

Open AccessArticle

Advantages of Liquid Nitrogen Quick Freezing Combine Gradient Slow Thawing for Quality Preserving of Blueberry

by Lina Cheng, Weijun Wu, Kejing An, Yujuan Xu, Yuanshan Yu, Jing Wen, Jijun Wu, Ying Zou, Haocheng Liu, Jieli Zhu and Gengsheng Xiao

Crystals 2020, 10(5), 368; https://doi.org/10.3390/cryst10050368 - 4 May 2020

Cited by 25 | Viewed by 5583

Abstract

Berries are perishable fruits with high nutritional value. Freezing is an effective way for food preservation. Freezing and thawing methods play key roles in preserving edible values and commodity values of food. This study investigated the effects of spray liquid nitrogen quick freezing (NF_{−20~−100 °C}) and gradient thawing on the physical and functional characteristics of blueberries by using immersion and refrigerator freezing and microwave, ultrasonic, room- and low-temperature, and static-water thawing as comparisons. The results show that NF_{−80 °C} freezing combined with −20~−5~4 °C. gradient thawing can retain more than 95% of polyphenols and other nutritional compounds (including pectin, soluble sugar, and vitamin C) in thawed blueberries compared with fresh blueberries. Besides, this method shows the best results in preserving the hardness, cell structure, and water distribution of blueberries. It is also revealed that the ultralow temperature (−100 °C) freezing does not bring a significant advantage in preserving blueberries. Rapid thawing methods such as microwave and ultrasound thawing are not suitable for blueberries, which might be due to their small size and thin skin. The results suggested that the combination of NF_{−80 °C} freezing and −20~−5~4 °C gradient thawing is the optimal process for blueberry preservation. The outcomes of this study will serve as theoretical guidance for improving the industrial process for freezing and thawing blueberries. Full article

(This article belongs to the Special Issue Ice Crystals)

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14 pages, 3691 KiB

Open AccessArticle

Appearance and Disappearance of Quasi-Liquid Layers on Ice Crystals in the Presence of Nitric Acid Gas

by Ken Nagashima, Josée Maurais, Ken-ichiro Murata, Yoshinori Furukawa, Patrick Ayotte and Gen Sazaki

Crystals 2020, 10(2), 72; https://doi.org/10.3390/cryst10020072 - 29 Jan 2020

Cited by 3 | Viewed by 3316

Abstract

The surfaces of ice crystals near the melting point are covered with thin liquid water layers, called quasi-liquid layers (QLLs), which play crucial roles in various chemical reactions in nature. So far, there have been many spectroscopic studies of such chemical reactions on ice surfaces, however, revealing the effects of atmospheric gases on ice surfaces remains an experimental challenge. In this study, we chose HNO₃ as a model atmospheric gas, and directly observed the ice basal faces by advanced optical microscopy under partial pressure of HNO₃ (~10⁻⁴ Pa), relevant to those found in the atmosphere. We found that droplets (HNO₃-QLLs) appeared on ice surfaces at temperatures ranging from −0.9 to −0.2 °C with an increase in temperature, and that they disappeared at temperatures ranging from −0.6 to −1.3 °C with decreasing temperature. We also found that the size of the HNO₃-QLLs decreased immediately after we started reducing the temperature. From the changes in size and the liquid–solid phase diagram of the HNO₃-H₂O binary system, we concluded that the HNO₃-QLLs did not consist of pure water, but rather aqueous HNO₃ solutions, and that the temperature and HNO₃ concentration of the HNO₃-QLLs also coincided with those along a liquidus line. Full article

(This article belongs to the Special Issue Ice Crystals)

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17 pages, 2925 KiB

Open AccessArticle

Dissociation Behavior of Dislocations in Ice

by Takeo Hondoh

Crystals 2019, 9(8), 386; https://doi.org/10.3390/cryst9080386 - 27 Jul 2019

Cited by 2 | Viewed by 4237

Abstract

Dislocations in ice behave very differently from those in other materials due to the very low energies of stacking faults in the ice basal plane. As a result, the dislocations dissociate on the basal plane, from a perfect dislocation into two partial dislocations with equilibrium width w_e ranging from 20 to 500 nm, but what is the timescale to reach this dissociated state? Using physical models, we estimate this timescale by calculating two time-constants: the dissociation-completing time t_d and the dissociation-beginning time t_b. These time constants are calculated for two Burgers vectors as a function of temperature. For perfect dislocations with Burgers vector <c + a>, t_d is more than one month even at the melting temperature T_M, and it exceeds 10³ years below −50 ℃, meaning that the dissociation cannot be completed during deformation over laboratory timescales. However, in this case the beginning time t_b is less than one second at T_M, and it is within several tens of minutes above −50 ℃. These dislocations can glide on non-basal planes until they turn to the dissociated state during deformation, finally resulting in sessile extended dislocations of various widths approaching to the equilibrium value w_e. In contrast, for perfect dislocations with Burgers vector <a>, t_d is less than one second above −50 ℃, resulting in glissile extended dislocations with the equilibrium width w_e on the basal plane. This width is sensitive to the shear stress τ exerted normal to the dislocation line, leading to extension of the intervening stacking fault across the entire crystal grain under commonly accessible stresses. Also, due to the widely dissociated state, dislocations <a> cannot cross-slip to non-basal planes. Such behavior of extended dislocations in ice are notable when compared to those of other materials. Full article

(This article belongs to the Special Issue Ice Crystals)

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15 pages, 4454 KiB

Open AccessArticle

Effect of Type I Antifreeze Proteins on the Freezing and Melting Processes of Cryoprotective Solutions Studied by Site-Directed Spin Labeling Technique

by Adiel F. Perez, Kyle R. Taing, Justin C. Quon, Antonia Flores and Yong Ba

Crystals 2019, 9(7), 352; https://doi.org/10.3390/cryst9070352 - 11 Jul 2019

Cited by 8 | Viewed by 4955

Abstract

Antifreeze proteins (AFPs) protect organisms living in subzero environments from freezing injury, which render them potential applications for cryopreservation of living cells, organs, and tissues. Cryoprotective agents (CPAs), such as glycerol and propylene glycol, have been used as ingredients to treat cellular tissues and organs to prevent ice crystal’s formation at low temperatures. To assess AFP’s function in CPA solutions, we have the applied site-directed spin labeling technique to a Type I AFP. A two-step process to prevent bulk freezing of the CPA solutions was observed by the cryo-photo microscopy, i.e., (1) thermodynamic freezing point depression by the CPAs; and (2) inhibition to the growth of seed ice crystals by the AFP. Electron paramagnetic resonance (EPR) experiments were also carried out from room temperature to 97 K, and vice versa. The EPR results indicate that the spin labeled AFP bound to ice surfaces, and inhibit the growths of ice through the bulk freezing processes in the CPA solutions. The ice-surface bound AFP in the frozen matrices could also prevent the formation of large ice crystals during the melting processes of the solutions. Our study illustrates that AFPs can play an active role in CPA solutions for cryopreservation applications. Full article

(This article belongs to the Special Issue Ice Crystals)

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14 pages, 2318 KiB

Open AccessArticle

Ice Crystal Coarsening in Ice Cream during Cooling: A Comparison of Theory and Experiment

by Jingyi Mo, Robert D. Groot, Graham McCartney, Enyu Guo, Julian Bent, Gerard van Dalen, Peter Schuetz, Peter Rockett and Peter D. Lee

Crystals 2019, 9(6), 321; https://doi.org/10.3390/cryst9060321 - 25 Jun 2019

Cited by 12 | Viewed by 5792

Abstract

Ice cream is a complex multi-phase structure and its perceived quality is closely related to the small size of ice crystals in the product. Understanding the quantitative coarsening behaviour of ice crystals will help manufacturers optimise ice cream formulations and processing. Using synchrotron X-ray tomography, we measured the time-dependent coarsening (Ostwald ripening) of ice crystals in ice cream during cooling at 0.05 °C/min. The results show ice crystal coarsening is highly temperature dependent, being rapid from ca. −6 to −12 °C but significantly slower at lower temperatures. We developed a numerical model, based on established coarsening theory, to calculate the relationship between crystal diameter, cooling rate and the weight fraction of sucrose in solution. The ice crystal diameters predicted by the model are found to agree well with the measured values if matrix diffusion is assumed to be slowed by a factor of 1.2 due to the presence of stabilizers or high molecular weight sugars in the ice cream formulation. Full article

(This article belongs to the Special Issue Ice Crystals)

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16 pages, 510 KiB

Open AccessArticle

Quasi-Liquid Layer on Ice and Its Effect on the Confined Freezing of Porous Materials

by Qiang Zeng and Kefei Li

Crystals 2019, 9(5), 250; https://doi.org/10.3390/cryst9050250 - 14 May 2019

Cited by 16 | Viewed by 3942

Abstract

Freezing of the water confined in thin pores can be destructive to the porous frame, but the effect of the quasi-liquid layer (QLL) between the confined ice and the pore walls remains still far from being fully understood. In the present study, the physical origins of the intermediate phase of QLL were discussed by thermodynamic analyses. Different interactions on QLL bring different models to estimate its thickness, which generally decays with temperature decreasing. Four representative models of QLL thickness were selected to unveil its effect on the growing rates and extents of ice in a concrete. The engineering consequences of the confined freezing were then discussed in the aspects of effective pore pressures built from the confined ice growth and deformations framed by a poro-elastic model. Overall, thickening QLL depresses ice growing rates and contents and, consequentially, decreases pore pressures and material deformations during freezing. The QLL corrections also narrow the gaps between the predicted and measured freezing deformations. The findings of this study contribute to profound understandings of confined freezing that may bridge over physical principles and engineering observations. Full article

(This article belongs to the Special Issue Ice Crystals)

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11 pages, 3667 KiB

Open AccessArticle

Negative Thermal Expansivity of Ice: Comparison of the Monatomic mW Model with the All-Atom TIP4P/2005 Water Model

by Muhammad Mahfuzh Huda, Takuma Yagasaki, Masakazu Matsumoto and Hideki Tanaka

Crystals 2019, 9(5), 248; https://doi.org/10.3390/cryst9050248 - 14 May 2019

Cited by 1 | Viewed by 3155

Abstract

We calculate the thermal expansivity of ice I for the monatomic mW model using the quasi-harmonic approximation. It is found that the original mW model is unable to reproduce the negative thermal expansivity experimentally observed at low temperatures. A simple prescription is proposed to recover the negative thermal expansion by re-adjusting the so-called tetrahedrality parameter, λ. We investigate the relation between the λ value and the Grüneisen parameter to explain the origin of negative thermal expansion in the mW model and compare it with an all-atom water model that allows the examination of the effect of the rotational motions on the volume of ice. Full article

(This article belongs to the Special Issue Ice Crystals)

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17 pages, 2723 KiB

Open AccessArticle

Decomposition Characterizations of Methane Hydrate Confined inside Nanoscale Pores of Silica Gel below 273.15 K

by Lihua Wan, Xuebing Zhou, Peili Chen, Xiaoya Zang, Deqing Liang and Jinan Guan

Crystals 2019, 9(4), 200; https://doi.org/10.3390/cryst9040200 - 10 Apr 2019

Cited by 11 | Viewed by 3906

Abstract

The formation and decomposition of gas hydrates in nanoscale sediments can simulate the accumulation and mining process of hydrates. This paper investigates the Raman spectra of water confined inside the nanoscale pores of silica gel, the decomposition characterizations of methane hydrate that formed from the pore water, and the intrinsic relationship between them. The results show that pore water has stronger hydrogen bonds between the pore water molecules at both 293 K and 223 K. The structure of pore water is conducive to the nucleation of gas hydrate. Below 273.15 K, the decomposition of methane hydrate formed from pore water was investigated at atmospheric pressure and at a constant volume vessel. We show that the decomposition of methane hydrate is accompanied by a reformation of the hydrate phase: The lower the decomposition temperature, the more times the reformation behavior occurs. The higher pre-decomposition pressure that the silica gel is under before decomposition is more favorable to reformation. Thus, reformation is the main factor in methane hydrate decomposition in nanoscale pores below 273.15 K and is attributed to the structure of pore water. Our results provide experimental data for exploring the control mechanism of hydrate accumulation and mining. Full article

(This article belongs to the Special Issue Ice Crystals)

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10 pages, 1868 KiB

Open AccessArticle

Collective Transformation of Water between Hyperactive Antifreeze Proteins: RiAFPs

by Kenji Mochizuki and Masakazu Matsumoto

Crystals 2019, 9(4), 188; https://doi.org/10.3390/cryst9040188 - 1 Apr 2019

Cited by 5 | Viewed by 2754

Abstract

We demonstrate, by molecular dynamics simulations, that water confined between a pair of insect hyperactive antifreeze proteins from the longhorn beetle Rhagium inquisitor is discontinuously expelled as the two proteins approach each other at a certain distance. The extensive striped hydrophobic–hydrophilic pattern on the surface, comprising arrays of threonine residues, enables water to form three independent ice channels through the assistance of hydroxyl groups, even at 300 K. The transformation is reminiscent of a freezing–melting transition rather than a drying transition and governs the stable protein–protein separation in the evaluation of the potential of mean force. The collectivity of water penetration or expulsion and the hysteresis in the time scale of ten nanoseconds predict a potential first-order phase transition at the limit of infinite size and provide a new framework for the water-mediated interaction between solutes. Full article

(This article belongs to the Special Issue Ice Crystals)

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9 pages, 1509 KiB

Open AccessArticle

Tetrahydrofuran (THF)-Mediated Structure of THF·(H₂O)_n_=1–10: A Computational Study on the Formation of the THF Hydrate

by Jinxiang Liu, Yujie Yan, Youguo Yan and Jun Zhang

Crystals 2019, 9(2), 73; https://doi.org/10.3390/cryst9020073 - 31 Jan 2019

Cited by 10 | Viewed by 6065

Abstract

Tetrahydrofuran (THF) is well known as a former and a promoter of clathrate hydrates, but the molecular mechanism for the formation of these compounds is not yet well understood. We performed ab initio calculations and ab initio molecular dynamics simulations to investigate the formation, structure, and stability of THF·(H₂O)_n_=1–10 and its significance to the formation of the THF hydrate. Weak hydrogen bonds were found between THF and water molecules, and THF could promote water molecules from the planar pentagonal or hexagonal ring. As a promoter, THF could increase the binding ability of the CH₄, CO₂, or H₂ molecule onto a water face, but could also enhance the adsorption of other THF molecules, causing an enrichment effect. Full article

(This article belongs to the Special Issue Ice Crystals)

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