Faster Nucleation of Ice at the Three-Phase Contact Line: Influence of Interfacial Chemistry
Faster Nucleation of Ice at the Three-Phase Contact Line: Influence of Interfacial Chemistry
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DOI：
10.1021/acs.langmuir.1c02044
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发表时间：
2021-10-25
期刊：
影响因子：
3.9
通讯作者：
Bahadur, Vaibhav
中科院分区：
文献类型：
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作者：
Kar, Aritra;Bhati, Awan;Bahadur, Vaibhav
控制冰成核在许多领域都很重要，包括大气科学、低温保存、食品科学和基础设施保护。目前，我们进行受控实验和分析，以揭示三相线表面化学对冰成核的影响。我们表明，用硅油和杏仁油等油替换水-空气界面处的空气后，冰成核速度更快。我们通过具有统计意义且精心设计的实验表明，与铝-水-空气界面相比，在铝-水-硅油（或杏仁油）界面处冰成核发生在更高的温度下。我们表明，可以通过控制三相线的界面化学来控制冰成核的位置（在冰成核多个位置的情况下）。我们开发了一个模型（利用经典成核理论）来研究两个界面对源自三相接触线的冰晶种的综合影响。该模型可以评估三相线成核与界面异质成核之间的热力学竞争。该模型表明，三相接触线通常会产生比异相成核更高的驱动力，从而加速成核动力学。总的来说，我们的实验和建模揭示了关于三相线对接触冷冻过程中成核的影响的一些有用的见解。
Controlling the nucleation of ice is important in many areas including atmospheric sciences, cryopreservation, food science, and infrastructure protection. Presently, we conduct controlled experiments and analysis to uncover the influence of surface chemistry at the three-phase line on ice nucleation. We show that ice nucleation is faster upon replacing the air at the water-air interface with oils like silicone oil and almond oil. We show via statistically meaningful and carefully designed experiments that ice nucleation occurs at a higher temperature at an aluminum-water-silicone oil (or almond oil) interface as compared to an aluminum-water-air interface. We show that the location of ice nucleation can be controlled (in situations with multiple locations for ice nucleation) by controlling the interfacial chemistry at the three-phase line. We develop a model (which utilizes classical nucleation theory) to study the combined influence of two interfaces on a seed crystal of ice originating at the three-phase contact line. This model can evaluate the thermodynamic competition between nucleation at the three-phase line and heterogeneous nucleation at an interface. The model shows that three-phase contact lines usually result in a higher driving force than heterogeneous nucleation, which speeds up nucleation kinetics. Overall, our experiments and modeling uncover several useful insights into the influence of three-phase lines on nucleation during contact freezing.