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中国物理学会期刊

水基有机溶剂液膜冻结初期表层冰片生长机制

CSTR: 32037.14.aps.74.20250902

Growth mechanism of surface ice flakes at the initial stage of freezing of water-based organic solvent liquid film

CSTR: 32037.14.aps.74.20250902
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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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