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Temperature-Dependent Phase Transitions of Aqueous Aerosol Droplet Systems in Microfluidic Traps
ACS Earth and Space Chemistry ( IF 2.9 ) Pub Date : 2020-08-20 , DOI: 10.1021/acsearthspacechem.0c00114
Priyatanu Roy 1 , Liora E. Mael 2 , Iaroslav Makhnenko 1 , Robert Martz 1 , Vicki H. Grassian 2 , Cari S. Dutcher 1, 3
Affiliation  

Well-mixed atmospheric aqueous aerosol droplets containing multiple chemical species can undergo processes such as liquid–liquid phase separation (LLPS) and crystallization depending on the ambient temperature and relative humidity (RH). So far, only a handful of single droplet studies have examined the effect of temperature in conjunction with the organic to inorganic ratio (OIR) on the separation RH for LLPS. In this work, we present a temperature-controlled microfluidic static trap approach to study the LLPS and efflorescence phenomenon in multiple ternary systems in a quasi-equilibrium manner. Ammonium sulfate or sodium chloride is used as the inorganic phase and 3-methylglutaric acid (3-MGA), poly(ethylene glycol), poly(propylene glycol), or poly(ethylene glycol) diacrylate is used as the organic phase. Results show a clear trend in droplets containing 3-MGA with either salt of the initial LLPS and efflorescence events occurring at higher RH at lower temperatures, while this trend is less obvious for the other organics. The organic to inorganic ratio (OIR) of the system also affected the type of first phase transition, which can be either LLPS or efflorescence. Finally, the rate of RH change also had an impact on the temperature dependence of the formation of either anhydrous or dihydrous crystals of sodium chloride upon efflorescence. These results help inform the effects of temperature, OIR, and rate of RH change on the phase state of aqueous aerosol droplets containing multiple species.

中文翻译:

微流阱中水雾液滴系统的温度相关相变

包含多种化学物质的大气混合气溶胶液滴的混合均匀,可能会经历液相-液相分离(LLPS)和结晶等过程,具体取决于环境温度和相对湿度(RH)。到目前为止,只有极少数的单滴研究检查了温度以及有机物与无机物的比率(OIR)对LLPS分离RH的影响。在这项工作中,我们提出一种温度控制的微流体静态阱方法,以准平衡的方式研究多三元系统中的LLPS和风化现象。硫酸铵或氯化钠用作无机相,3-甲基戊二酸(3-MGA),聚乙二醇,聚丙二醇或聚乙二醇二丙烯酸酯用作有机相。结果显示,含有3-MGA的液滴具有明显的趋势,初始LLPS的盐和风化事件均发生在较高的RH和较低的温度下,而其他有机物的趋势则不太明显。系统的有机无机比(OIR)也影响第一相变的类型,可以是LLPS或风化。最后,相对湿度的变化速率也对风化时氯化钠无水或二水氯化钠晶体形成的温度依赖性产生影响。这些结果有助于告知温度,OIR和RH变化率对包含多种物质的气溶胶液滴的相态的影响。而对于其他有机物,这种趋势不太明显。系统的有机无机比(OIR)也影响第一相变的类型,可以是LLPS或风化。最后,相对湿度的变化速率也对风化后氯化钠无水或二水氯化钠晶体形成的温度依赖性产生影响。这些结果有助于告知温度,OIR和RH变化率对包含多种物质的气溶胶液滴的相态的影响。而对于其他有机物,这种趋势不太明显。系统的有机无机比(OIR)也影响第一相变的类型,可以是LLPS或风化。最后,相对湿度的变化速率也对风化时氯化钠无水或二水氯化钠晶体形成的温度依赖性产生影响。这些结果有助于告知温度,OIR和RH变化率对包含多种物质的气溶胶液滴的相态的影响。RH变化的速率也对风化后形成无水或二水氯化钠晶体的温度依赖性产生影响。这些结果有助于告知温度,OIR和RH变化率对包含多种物质的气溶胶液滴的相态的影响。RH变化的速率也对风化后形成氯化钠无水或二水晶体的温度依赖性产生影响。这些结果有助于告知温度,OIR和RH变化率对包含多种物质的气溶胶液滴的相态的影响。
更新日期:2020-09-18
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