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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Kinetic Limitation to Inorganic Ion Diffusivity and to Coalescence of Inorganic Inclusions in Viscous Liquid-Liquid Phase-Separated Particles
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Kinetic Limitation to Inorganic Ion Diffusivity and to Coalescence of Inorganic Inclusions in Viscous Liquid-Liquid Phase-Separated Particles

机译：对无机离子扩散性的动力学限制和粘性液 - 液相分离颗粒中无机夹杂物的聚结

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摘要

Mixed organic/inorganic aerosols may undergo liquid-liquid phase separation (LLPS) when the relative humidity drops in the atmosphere. Phase-separated particles adopt different morphologies, which will have different consequences for atmospheric chemistry and climate. Recent laboratory studies on submicron particles led to speculation whether LLPS observed for larger drops might actually be suppressed in smaller droplets. Here, we report on micron-sized droplets of a ternary mixture of ammonium sulfate (AS), carminic acid, and water at different temperatures, which were exposed to typical atmospheric drying rates ranging from 0.34 to 5.0% RH min(-1). Our results reveal that increasing the drying rate and lowering the temperature results in different morphologies after LLPS and may suppress the growth and coalescence of the inorganic-rich phase inclusions due to kinetic limitations in a viscous matrix. The coalescence time was used to estimate the viscosity of the organic-rich phase within a factor of 20, and based on the Stokes-Einstein relationship, we estimated AS diffusivity. Furthermore, we evaluated the initial growth of inclusions to quantitatively determine the AS diffusivity in the organic-rich phase, which is about 10(-8) cm(2) s(-1) at room temperature. Extrapolation of diffusivity to lower temperatures using estimations for the diffusion activation energy leads us to conclude that the growth of the inorganic phase is not kinetically impeded for tropospheric submicron particles larger than 100 nm.
机译：当在大气中相对湿度下降时，混合有机/无机气溶胶可能经历液 - 液相分离（LLP）。相分离的颗粒采用不同的形态，这将对大气化学和气候产生不同的后果。最近对亚微米粒子的实验室研究导致猜测对于较大的液滴观察到LLP是否实际上可能在较小的液滴中抑制。在此，我们在不同温度下报告硫酸铵（AS），甘氨酸和水的三元混合物的微米尺寸液滴，其暴露于0.34-5.0％RH min（-1）的典型大气干燥速率。我们的结果表明，在LLP之后增加干燥速率并降低温度导致不同的形态，并且由于粘性基质中的动力学限制，可以抑制富含无机相夹杂物的生长和聚结。聚结时间用于估计20倍，基于斯托克斯 - 爱因斯坦关系的富股，我们估计是扩散性。此外，我们评估了夹杂物的初始生长，以定量地确定在室温下为约10（-8）cm（2）厘米（2）厘米（2）厘米（2）厘米（-1）的扩散率。使用扩散活化能的估计的扩散率的外推导致我们得出结论，无机相的生长不是用于大于100nm的对流层亚微米粒子的动力学。

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