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Crossover from lamellar to spongy ice morphologies within a single ice crystal during unidirectional freezing of an aqueous solution

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 Added by Tongxin Zhang
 Publication date 2021
  fields Physics
and research's language is English




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Ice growth from liquid phase has been extensively investigated in various conditions, especially for ice freely grown in undercooled water and aqueous solutions. Although unidirectional ice growth plays a significant role in sea ice and freeze casting, the detailed pattern formation of unidirectionally grown ice in an aqueous solution remains elusive. For the first time, we in situ proved a crossover from lamellar to spongy ice morphologies of a single ice crystal via unidirectional freezing of an aqueous solution. The spongy ice morphology originates from the intersect of tilted lamellar ice and is observed in a single ice crystal, which is intrinsically different from the competitive growth of bi-crystal composed of two differently orientated grains in directional solidification. These results provide a complete physical picture of unidirectionally grown ice from aqueous solution and are believed to promote our understanding of various pattern of ice in many relevant domains where pattern formation of ice crystal is vital.

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Freezing of ice has been largely reported from many aspects, especially its complex pattern formation. Ice grown from liquid phase is usually characteristic of lamellar morphology which plays a significant role in various domains. However, tilted growth of ice via transition from coplanar to non-coplanar growth in directional solidification has been paid little attention in previous studies and there is misleading explanation of the formation of tilted lamellar ice. Here, we in-situ investigated the variations of tilting behavior of lamellar ice tip under different conditions within a single ice crystal with manipulated orientation via unidirectional freezing of aqueous solutions. It is found that tilted growth of ice tips is sensitive to pulling velocity and solute type. These experimental results reveal intrinsic tilted growth behavior of lamellar ice and enrich our understanding in pattern formation of ice.
Ice growth has attracted great attention for its capability of fabricating hierarchically porous microstructure. However, the formation of tilted lamellar microstructure during freezing needs to be reconsidered due to the limited control of ice orientation with respect to thermal gradient during in-situ observations, which can greatly enrich our insight into architectural control of porous biomaterials. This paper provides an in-situ study of solid/liquid interface morphology evolution of directionally solidified single crystal ice with its C-axis (optical axis) perpendicular to directions of both thermal gradient and incident light in poly (vinyl alcohol, PVA) solutions. Misty morphology and V-shaped lamellar morphology were clearly observed in-situ for the first time. Quantitative characterizations on lamellar spacing, tilt angle and tip undercooling of lamellar ice platelets provide a clearer insight into the inherent ice growth habit in polymeric aqueous systems and are suggested exert significant impact on future design and optimization in porous biomaterials.
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