The Many Faces of Heterogeneous Ice Nucleation: Interplay Between Surface Morphology and Hydrophobicity

Fitzner, Martin; Sosso, Gabriele C.; Cox, Stephen J.; Michaelides, Angelos

doi:10.1021/jacs.5b08748

Cited by 204 publications

(304 citation statements)

References 131 publications

(366 reference statements)

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“…Our experiments show that only when synergetic cooperation of specific spatial arrangement of methyl groups (hydrophobic) and hydroxyl groups (hydrophilic) can lead to a pronounced promotion of ice nucleation (in the case of MpdAFP and MpAFP), whereas arrangement of merely hydroxyl groups leads to a modest or no obvious promotion of ice nucleation (type III AFP). These results obviously show that hydrophobicity is not the criterion for predicting the heterogeneous ice nucleation capacity of a surface, which is also recently suggested by some theoretical research groups (35,47,48). In combining with the MD simulation analysis, our work shows that the structure of interfacial water atop a specific solid surface, i.e., if it can facilitate the epitaxial growth of ice crystals, may be a good criterion for predicting the ice nucleation capability of this surface.…”

Section: Discussionsupporting

confidence: 55%

“…On the NIBF, irregular arrangement of hydrophobic/ hydrophilic groups and the existence of bulky hydrophobic groups and charged groups lead to the disordered structure. Depending on previous reports (35,39,40), the fraction of ice-like water molecules determines ice nucleation. This means that the IBF with hexagonal ice-like structured hydration layer promotes ice nucleation and the NIBF with disordered hydration layer depresses ice nucleation (41,42), which are consistent with our experimental observations.…”

Section: Significancementioning

confidence: 97%

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Janus effect of antifreeze proteins on ice nucleation

Liu

Wang

et al. 2016

Proc. Natl. Acad. Sci. U.S.A.

241

187

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The mechanism of ice nucleation at the molecular level remains largely unknown. Nature endows antifreeze proteins (AFPs) with the unique capability of controlling ice formation. However, the effect of AFPs on ice nucleation has been under debate. Here we report the observation of both depression and promotion effects of AFPs on ice nucleation via selectively binding the ice-binding face (IBF) and the non-ice-binding face (NIBF) of AFPs to solid substrates. Freezing temperature and delay time assays show that ice nucleation is depressed with the NIBF exposed to liquid water, whereas ice nucleation is facilitated with the IBF exposed to liquid water. The generality of this Janus effect is verified by investigating three representative AFPs. Molecular dynamics simulation analysis shows that the Janus effect can be established by the distinct structures of the hydration layer around IBF and NIBF. Our work greatly enhances the understanding of the mechanism of AFPs at the molecular level and brings insights to the fundamentals of heterogeneous ice nucleation.antifreeze proteins | ice nucleation | Janus effect | interfacial water | selective tethering A ntifreeze proteins (AFPs) protect a broad range of organisms inhabiting subzero environments. The function of AFPs lies in lowering the freezing point in a noncolligative manner (1, 2). It has been shown that AFPs can adsorb on the ice crystal surface with the ice-binding face (IBF, also termed ice-binding site or icebinding surface) (3, 4). The adsorbed AFPs lead to curvatures on the ice surface between adjacent AFPs, and ice growth is retarded due to the Kelvin effect, which is known as the adsorptioninhibition mechanism (5). However, whether the non-ice-binding face (NIBF) is involved in the function of AFPs and what effect the NIBF exerts are rarely studied (4, 6, 7). On the other hand, the effect of AFPs on ice nucleation (8) is still under intense debate (9-13), although ice nucleation, the formation of a stable nucleus with a critical size, is the control step for ice formation (8). Liu et al. (9) suggested that AFPs could inhibit heterogeneous ice nucleation of water, whereas research on ice nucleation of microdroplets of AFP solutions exhibited no obvious effect of AFPs in inhibiting ice nucleation (10). It was also reported that an AFP solution with high concentration facilitated ice nucleation (11). The contradiction also exists for the research of ice nucleation on solid surfaces immobilized with AFPs (12, 13). Therefore, it is highly desirable to elucidate the exact role of AFPs on ice nucleation and to correlate AFP structures at the molecular level with their function in tuning ice nucleation, which is essential for practical applications in food, pharmaceutical, and chemical industries (14,15).Herein, we investigate the effect of IBF and NIBF of AFPs on ice nucleation via binding AFPs to solid substrates in a way that either IBF or NIBF is exposed to liquid water. This binding method is readily extendable to other AFPs because of the clear distinction...

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Section: Discussionsupporting

confidence: 55%

Section: Significancementioning

confidence: 97%

Janus effect of antifreeze proteins on ice nucleation

Liu

Wang

et al. 2016

Proc. Natl. Acad. Sci. U.S.A.

241

187

View full text Add to dashboard Cite

show abstract

“…Therefore, he suggested that the site for heterogeneous ice nucleation does not have to be ordered or, more particularly, does not have to possess a hexagonal geometry to match the structure of Ih. In a molecular dynamics study, Fitzner et al (2015) found that lattice match is at most desirable but not a requirement for heterogeneous ice nucleation.…”

Section: Lattice Match and Surface Chargementioning

confidence: 99%

Ice nucleation efficiency of AgI: review and new insights

et al. 2016

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Abstract. AgI is one of the best-investigated ice-nucleating substances. It has relevance for the atmosphere since it is used for glaciogenic cloud seeding. Theoretical and experimental studies over the last 60 years provide a complex picture of silver iodide as an ice-nucleating agent with conflicting and inconsistent results. This review compares experimental ice nucleation studies in order to analyze the factors that influence the ice nucleation ability of AgI. The following picture emerges from this analysis: the ice nucleation ability of AgI seems to be enhanced when the AgI particle is on the surface of a droplet, which is indeed the position that a particle takes when it can freely move in a droplet. The ice nucleation by particles with surfaces exposed to air depends on water adsorption. AgI surfaces seem to be most efficient at nucleating ice when they are exposed to relative humidity at or even above water saturation. For AgI particles that are completely immersed in water, the freezing temperature increases with increasing AgI surface area. Higher threshold freezing temperatures seem to correlate with improved lattice matches as can be seen for AgI-AgCl solid solutions and 3AgI q NH 4 I q 6H 2 O, which have slightly better lattice matches with ice than AgI and also higher threshold freezing temperatures. However, the effect of a good lattice match is annihilated when the surfaces have charges. Also, the ice nucleation ability seems to decrease during dissolution of AgI particles. This introduces an additional history and time dependence for ice nucleation in cloud chambers with short residence times.

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“…Hu and Michaelides, 2007;Cox et al, 2012;Reinhardt and Doye, 2014;Zielke et al, 2015;Cox et al, 2015a, b;Fitzner et al, 2015;Pedevilla et al, 2016). To date there has been little overlap between work of this nature and laboratory experiments.…”

Section: Introductionmentioning

confidence: 99%

Not all feldspars are equal: a survey of ice nucleating properties across the feldspar group of minerals

et al. 2016

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Abstract. Mineral dust particles from wind-blown soils are known to act as effective ice nucleating particles in the atmosphere and are thought to play an important role in the glaciation of mixed phase clouds. Recent work suggests that feldspars are the most efficient nucleators of the minerals commonly present in atmospheric mineral dust. However, the feldspar group of minerals is complex, encompassing a range of chemical compositions and crystal structures. To further investigate the ice-nucleating properties of the feldspar group we measured the ice nucleation activities of 15 characterized feldspar samples. We show that alkali feldspars, in particular the potassium feldspars, generally nucleate ice more efficiently than feldspars in the plagioclase series which contain significant amounts of calcium. We also find that there is variability in ice nucleating ability within these groups. While five out of six potassium-rich feldspars have a similar ice nucleating ability, one potassium rich feldspar sample and one sodium-rich feldspar sample were significantly more active. The hyper-active Na-feldspar was found to lose activity with time suspended in water with a decrease in mean freezing temperature of about 16 • C over 16 months; the mean freezing temperature of the hyper-active K-feldspar decreased by 2 • C over 16 months, whereas the "standard" K-feldspar did not change activity within the uncertainty of the experiment. These results, in combination with a review of the available literature data, are consistent with the previous findings that potassium feldspars are important components of arid or fertile soil dusts for ice nucleation. However, we also show that there is the possibility that some alkali feldspars may have enhanced ice nucleating abilities, which could have implications for prediction of ice nucleating particle concentrations in the atmosphere.

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The Many Faces of Heterogeneous Ice Nucleation: Interplay Between Surface Morphology and Hydrophobicity

Cited by 204 publications

References 131 publications

Janus effect of antifreeze proteins on ice nucleation

Janus effect of antifreeze proteins on ice nucleation

Ice nucleation efficiency of AgI: review and new insights

Not all feldspars are equal: a survey of ice nucleating properties across the feldspar group of minerals

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