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水在三甘醇水溶液液滴上的质量容纳系数出人意料的浓度依赖性。

Unexpected concentration dependence of the mass accommodation coefficient of water on aqueous triethylene glycol droplets.

作者信息

Gleichweit Michael J, Azizbaig Mohajer Mercede, Borgeaud Dit Avocat Dominique P, Divéky Matúš E, David Grégory, Signorell Ruth

机构信息

Department of Chemistry and Applied Biosciences, ETH Zurich, CH-8093 Zurich, Switzerland.

出版信息

Phys Chem Chem Phys. 2024 Jun 6;26(22):16296-16308. doi: 10.1039/d4cp00966e.

Abstract

The mass accommodation coefficient of water on aqueous triethylene glycol droplets was determined for water mole fractions in the range = 0.1-0.93 and temperatures between 21 and 26 °C from modulated Mie scattering measurement on single optically-trapped droplets in combination with a kinetic multilayer model. reaches minimum values around 0.005 at a critical water concentration of = 0.38, and increases with decreasing water content to a value of ≈0.1 for almost pure triethylene glycol droplets, essentially independent of the temperature. Above = 0.38, first increases with increasing water content and then stabilises at a value of ≈0.1 at the lowest temperatures, while at the highest temperature its value remains around 0.005. We analysed the unexpected concentration and temperature dependence with a previously proposed two-step model for mass accommodation which provides concentration and temperature-dependent activation enthalpies and entropies. We suggest that the unexpected minimum in at intermediate water concentrations might arise from a more or less saturated hydrogen-bond network that forms at the droplet surface.

摘要

通过对单个光阱捕获液滴进行调制米氏散射测量,并结合动力学多层模型,测定了水在含水三甘醇液滴上的质量容纳系数,测量范围为水的摩尔分数(x_w = 0.1 - 0.93),温度在(21)至(26)°C之间。在临界水浓度(x_w = 0.38)时,质量容纳系数(α)达到最小值,约为(0.005),并且随着含水量的降低而增加,对于几乎纯的三甘醇液滴,(α)的值约为(0.1),基本与温度无关。在(x_w > 0.38)时,(α)首先随着含水量的增加而增加,然后在最低温度下稳定在约(0.1)的值,而在最高温度下其值保持在约(0.005)。我们用先前提出的两步质量容纳模型分析了这种意外的浓度和温度依赖性,该模型提供了与浓度和温度相关的活化焓和熵。我们认为,在中等水浓度下(α)出现意外最小值可能是由于在液滴表面形成了或多或少饱和的氢键网络。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/227a/11154172/4bc903f1127c/d4cp00966e-f1.jpg

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