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液滴及液膜冻结广泛存在于自然界与工程应用中, 近年多组分液滴体系已揭示界面流动与溶质再分布的普遍机制. 然而, 液滴界面曲率与视场限制使对单个分离冰片的连续显微原位观测受限. 鉴于液滴与液膜在冻结过程中的界面传热与溶质传输机理具有相似性, 本文采用平坦多组分液膜体系, 观察在冷表面上对异丙醇-水二元液膜在不同过冷度下的冻结过程, 开展对单个分离冰片的显微原位研究. 实验发现冰片外形随过冷度由六棱锥逐渐转变为十二棱锥和圆锥形, 并伴随透明度下降. 建立了考虑溶质扩散、热扩散与马兰戈尼效应的物理模型, 揭示了冰片形貌变化的主导机制. 结果表明, 冰片结构演化受溶质浓度梯度主导, 流动与扩散的竞争控制其各向异性生长特征. 本文为多组分液膜冻结过程中的界面动力学提供了新见解.Freezing of multicomponent droplets and thin films is ubiquitous in natural environments and engineered settings. Previous studies on multicomponent droplets, including Marangoni-driven self-lifting droplets and soap-bubble freezing, have identified the roles of interfacial flow and solute redistribution, often exhibiting a snow-globe effect of migrating ice particles. Curvature and field-of-view constraints in droplet systems hinder continuous observation of a single object. Here, utilizing the comparability of interfacial heat and mass transfer between droplets and films, we employ a flat isopropanol-water binary film on a cooled substrate to achieve high-resolution, time-resolved in-situ microscopy observation of individual separated ice flakes within a supercooling (ΔT) range of the substrate. Experiments show that with the increase of ΔT, the external shape of ice flakes evolves from hexagonal pyramid to dodecagonal pyramid and ultimately to a nearly-conical form, accompanied by the decrease of transparency. We quantify morphological evolution by using a shape factor β and qualitatively distinguish crystal-structure differences by combining bright-field and dark-field microscopy. A minimal model that couples solute and thermal diffusion with Marangoni stress rationalizes the observations: solute-concentration gradients primarily drive structural evolution, while the competition between advection and diffusion governs anisotropic growth. These results provide mechanistic insight into interfacial freezing dynamics of multi-component liquid films and establish flat-film microscopy as a platform for single-flake kinetics.
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Keywords:
- binary liquid film /
- solute diffusion /
- thermal diffusion /
- Marangoni effect
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图 1 (a) 实验装置示意图; (b) 硅片处理前后接触角对比; (c) $\Delta T = \left( {5.5 \pm 0.1} \right)$ ℃时异丙醇-水液膜冻结过程; (d), (e) 对单个冰片的显微观察的时间起点和终点
Fig. 1. (a) Schematic diagram of the experimental setup; (b) comparison of contact angles before and after plasma treatment of monocrystalline silicon wafers; (c) freezing process of isopropanol-water liquid film at $\Delta T = \left( {5.5 \pm 0.1} \right)$ ℃; (d), (e) the beginning and ending of microscopic observation of a single ice flake.
图 2 (a), (b) 不同过冷度下冰片生长动力学过程 (a) $\Delta T = \left( {4.1 \pm 0.1} \right)$ ℃; (b) $\Delta T = \left( {12.6 \pm 0.1} \right)$ ℃. (c), (d) 不同过冷度下冰片轮廓的变化 (c) $\Delta T = \left( {4.1 \pm 0.1} \right)$ ℃; (d) $\Delta T = \left( {12.6 \pm 0.1} \right)$ ℃
Fig. 2. (a), (b) Kinetic processes of ice flakes growth at different supercooling degrees: (a) $\Delta T = \left( {4.1 \pm 0.1} \right)$ ℃; (b) $\Delta T = $$ \left( {12.6 \pm 0.1} \right)$ ℃; (c), (d) Changes of ice flake profiles at different supercooling degrees: (c) $\Delta T = \left( {4.1 \pm 0.1} \right)$ ℃; (d) $\Delta T = $$ \left( {12.6 \pm 0.1} \right)$ ℃.
图 3 明场以及暗场观察对比 (a) 明场观察示意图; (b) 暗场观察示意图; (c) $\Delta T = \left( {4.1 \pm 0.1} \right)$ ℃暗场下无法观察到冰片, 冰片几乎透明; (d) $\Delta T = \left( {12.6 \pm 0.1} \right)$ ℃暗场下观察到冰片为白色且不透明
Fig. 3. Comparison of bright-field as well as dark-field observation: (a) Schematic of bright-field observation; (b) schematic of dark-field observation; (c) ice flakes could not be observed in the dark-field at $\Delta T = \left( {4.1 \pm 0.1} \right)$ ℃, and the ice flakes were almost transparent; (d) ice flakes were observed to be white and opaque in the dark-field at $\Delta T = \left( {12.6 \pm 0.1} \right)$ ℃.
图 4 (a) 不同过冷度下分离冰片形貌; (b) 形状因子定义; (c) 形状因子随过冷度变化规律
Fig. 4. (a) Morphology of separated ice flakes at different supercooling degrees; (b) definition of shape factor; (c) variation rule of shape factor with supercooling degree.
图 5 物理机制示意图 (a) 低过冷度下结冰偏析与马兰戈尼流的产生; (b) 过冷度增加溶质扩散减弱, 浓度差增加马兰戈尼流增强, 冰片加速生长; (c) 大过冷度下马兰戈尼流减弱导致溶质富集
Fig. 5. Schematic diagram of the physical mechanism: (a) Icing segregation and production of Marangoni flow at low subcooling; (b) weakened solute diffusion, enhanced Marangoni flow, and accelerated growth of ice flakes at increasing subcooling; (c) weakened Marangoni flow at large subcooling leading to solute enrichment.
图 6 (a) 冰片水平方向生长速度定义; (b) 冰片水平方向生长速度随过冷度变化
Fig. 6. (a) Definition of the horizontal growth velocity of the ice flakes; (b) horizontal growth velocity versus supercooling.
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