A kinetic partitioning method for simulating the condensation mass flux of organic vapors in a wide volatility range

IF 3.9 3区 环境科学与生态学 Q2 ENGINEERING, CHEMICAL Journal of Aerosol Science Pub Date : 2024-05-18 DOI:10.1016/j.jaerosci.2024.106400
Yuyang Li , Runlong Cai , Rujing Yin , Xiaoxiao Li , Yi Yuan , Zhaojin An , Junchen Guo , Dominik Stolzenburg , Markku Kulmala , Jingkun Jiang
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Abstract

Organic aerosols are ubiquitous, playing important roles in various atmospheric physicochemical processes such as the formation of cloud droplets and haze. Condensation of organic vapors, as a net effect of association with particles and dissociation from the condensed phase, is a fundamental process that drives the formation of organic aerosols. Kinetic models are often used to simulate the condensation fluxes of low-volatility organic vapors and aerosol growth. However, the widely used kinetic growth models usually calculate the evaporation of a certain species based on previous particulate compositions, without including the co-condensation of other species. Here we present a new kinetic partitioning method for calculating the condensation fluxes of organic vapors in a wide volatility range with low computational cost. In this method, the organic vapors are assumed to be in a quasi-steady state, but never reach real association-dissociation equilibrium during the simultaneous condensation of multiple species. We show a good consistency between the kinetic partitioning method and kinetic models in simulating particle mass fractions and condensation fluxes. Under relevant atmospheric conditions, we reveal that the kinetic partitioning method also reproduce the trend that low-volatility species are almost non-volatile while volatile organic compounds almost reach association-dissociation equilibrium, while there is a transition regime between them. This transition regime varies with atmospheric conditions, such as temperature and vapor concentrations. Compared with previous studies combining kinetic growth methods with equilibrium partitioning theories to simplify the condensation flux calculation, this method helps to improve accuracy without a significant expense of computation cost, and it can be applied in a wider range of atmospheric conditions such as in extremely cold atmospheres and polluted exhaust plumes.

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模拟宽挥发性范围内有机蒸汽冷凝质量通量的动力学分配法
有机气溶胶无处不在,在形成云滴和烟雾等各种大气物理化学过程中发挥着重要作用。有机蒸汽的凝结是与颗粒物结合和从凝结相解离的净效应,是推动有机气溶胶形成的基本过程。动力学模型通常用于模拟低挥发性有机蒸汽的凝结通量和气溶胶的生长。然而,广泛使用的动力学增长模型通常是根据之前的颗粒成分来计算某一物种的蒸发量,而不包括其他物种的共冷凝。在这里,我们提出了一种新的动力学分区方法,用于计算宽挥发性范围内有机蒸气的冷凝通量,计算成本较低。在这种方法中,有机蒸气被假定处于准稳态,但在多个物种同时冷凝的过程中永远不会达到真正的结合-解离平衡。在模拟颗粒质量分数和凝结通量时,我们发现动力学分区法与动力学模型之间具有良好的一致性。在相关大气条件下,我们发现动力学分配法也再现了低挥发性物种几乎不挥发,而挥发性有机化合物几乎达到缔合-解离平衡的趋势,而两者之间存在一个过渡机制。这种过渡机制随温度和蒸汽浓度等大气条件的变化而变化。与以往为简化冷凝通量计算而将动力学增长方法与平衡分配理论相结合的研究相比,该方法有助于在不大幅增加计算成本的情况下提高精确度,而且可以应用于更广泛的大气条件,如极冷大气和污染废气羽流。
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来源期刊
Journal of Aerosol Science
Journal of Aerosol Science 环境科学-工程:化工
CiteScore
8.80
自引率
8.90%
发文量
127
审稿时长
35 days
期刊介绍: Founded in 1970, the Journal of Aerosol Science considers itself the prime vehicle for the publication of original work as well as reviews related to fundamental and applied aerosol research, as well as aerosol instrumentation. Its content is directed at scientists working in engineering disciplines, as well as physics, chemistry, and environmental sciences. The editors welcome submissions of papers describing recent experimental, numerical, and theoretical research related to the following topics: 1. Fundamental Aerosol Science. 2. Applied Aerosol Science. 3. Instrumentation & Measurement Methods.
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