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颗粒粘度和颗粒相反应对二次有机气溶胶形成的物种特异性影响。

Species-specific effect of particle viscosity and particle-phase reactions on the formation of secondary organic aerosol.

作者信息

Luo Zekun, Zang Han, Li Ziyue, Li Chenxi, Zhao Yue

机构信息

School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240, China.

School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240, China; State Environmental Protection Key Laboratory of Formation and Prevention of the Urban Air Pollution Complex, Shanghai Academy of Environment Sciences, Shanghai 200233, China.

出版信息

Sci Total Environ. 2024 Nov 10;950:175207. doi: 10.1016/j.scitotenv.2024.175207. Epub 2024 Aug 2.

Abstract

Secondary organic aerosol (SOA) is a major component of atmospheric fine particulate matter. Both particle viscosity and particle-phase chemistry play a crucial role in the formation and evolution of SOA; however, our understanding on how these two factors together with gas-phase chemistry collectively determine the formation of SOA is still limited. Here we developed a kinetic aerosol multilayer model coupled with gas-phase and particle-phase chemistry to simulate SOA formation. We take the atmospherically important α-pinene + OH oxidation system as an example application of the model. The simulations show that although the particle viscosity has negligible to small influences on the total SOA mass concentration, it strongly changes the concentration and distribution of individual compounds within the particle. This complicated effect of particle viscosity on SOA formation is a combined result of inhibited condensation or evaporation of specific organics due to slowed particle-phase diffusion. Furthermore, the particle-phase reactions alter the volatility and abundance of specific compounds and exacerbate their non-uniform distribution in highly viscous particles. Our results highlight an important species-specific effect of particle viscosity and particle-phase chemistry on SOA formation and demonstrate the capability of our model for quantifying such complicated effects on SOA formation and evolution.

摘要

二次有机气溶胶(SOA)是大气细颗粒物的主要成分。颗粒粘度和颗粒相化学在SOA的形成和演化过程中都起着关键作用;然而,我们对于这两个因素如何与气相化学共同决定SOA的形成的理解仍然有限。在此,我们开发了一个结合气相和颗粒相化学的动力学气溶胶多层模型来模拟SOA的形成。我们以大气中重要的α-蒎烯+OH氧化体系为例对该模型进行应用。模拟结果表明,尽管颗粒粘度对SOA总质量浓度的影响可忽略不计或影响较小,但它会强烈改变颗粒内单个化合物的浓度和分布。颗粒粘度对SOA形成的这种复杂影响是由于颗粒相扩散减慢导致特定有机物的凝结或蒸发受到抑制的综合结果。此外,颗粒相反应改变了特定化合物的挥发性和丰度,并加剧了它们在高粘性颗粒中的非均匀分布。我们的结果突出了颗粒粘度和颗粒相化学对SOA形成的重要的物种特异性影响,并证明了我们的模型能够量化对SOA形成和演化的这种复杂影响。

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