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Maxwell–Stefan diffusion: a framework for predicting condensed phase diffusion and phase separation in atmospheric aerosol

机译:Maxwell-Stefan扩散:用于预测大气气溶胶中凝聚相扩散和相分离的框架

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The composition of atmospheric aerosol particles has been found to influence their micro-physical properties and their interaction with water vapour in the atmosphere. Core–shell models have been used to investigate the relationship between composition, viscosity and equilibration timescales. These models have traditionally relied on the Fickian laws of diffusion with no explicit account of non-ideal interactions. We introduce the Maxwell–Stefan diffusion framework as an alternative method, which explicitly accounts for non-ideal interactions through activity coefficients. e-folding time is the time it takes for the difference in surface and bulk concentration to change by an exponential factor and was used to investigate the interplay between viscosity and solubility and the effect this has on equilibration timescales within individual aerosol particles. The e-folding time was estimated after instantaneous increases in relative humidity to binary systems of water and an organic component. At low water mole fractions, viscous effects were found to dominate mixing. However, at high water mole fractions, equilibration times were more sensitive to a range in solubility, shown through the greater variation in e-folding times. This is the first time the Maxwell–Stefan framework has been applied to an atmospheric aerosol core–shell model and shows that there is a complex interplay between the viscous and solubility effects on aerosol composition that requires further investigation.
机译:已发现大气气溶胶颗粒的组成来影响其微观物理性质及其与大气中水蒸气的相互作用。核心壳模型已被用于研究成分,粘度和平衡时间尺度之间的关系。这些模型传统上依赖于Fickian的扩散定律,没有明确的非理想相互作用。我们将Maxwell-Stefan扩散框架介绍为替代方法,该方法明确地通过活动系数显式占非理想交互。 E折叠时间是表面和批量浓度差异变化的差异,用于研究粘度和溶解度之间的相互作用,并且这对各个气溶胶颗粒内的均衡时间造成的效果。在水和有机组分的相对湿度瞬时增加之后估计e折叠时间。在低水摩尔分数下,发现粘性效应占主导地位混合。然而,在高水摩尔分数下,平衡时间对溶解度的范围更敏感,通过电子折叠时间的更大变化示出。这是Maxwell-Stefan框架首次应用于大气气溶胶核心壳模型,并表明在需要进一步调查的气溶胶组合物对气溶胶组合物之间存在复杂的相互作用。

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