α-蒎烯与辛烯衍生的二级有机气溶胶的气粒分配和粘度特性

Qiaorong Xie, Sepehr Nikkho, Zoë M. Golay, Isaac S. Morton, Emily R. Halpern, Robert VanGundy, Alla Zelenyuk, Manish Shrivastava, Rahul A. Zaveri, Allan K. Bertram and Alexander Laskin*, 
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引用次数: 0

摘要

二次有机气溶胶(SOA)具有复杂的多组分组成,控制着颗粒粘度和气体-颗粒分配,这是其大气演变的关键因素。本研究考察了臭氧分解环α-蒎烯(PSOA)和无环辛烯(OSOA)单萜形成的SOA的化学组成、挥发性和粘度。使用程序升温解吸结合实时电离直接分析和高分辨率质谱,我们确定了单个SOA组分的分子组成和饱和质量浓度。这些数据可以在不同的大气条件下进行气粒分配和粘度估计。PSOA具有较高的分子量和较少的氧化组分,在高总有机质量(tOM)负载下具有较高的可缩聚性和粘度。相比之下,氧化程度更高、分子量更低的OSOA对tOM更敏感,稀释后粘度显著增加。Poke-flow实验支持这一趋势,表明OSOA在大气老化过程中经历了更动态的成分和相变化。这些观测结果揭示了环萜和非环萜在大气转化和SOA反应性方面的明显动态趋势,后者在老化过程中表现出更大的成分变化,从而改变了粘度和扩散。这突出了将这种动态转换合并到大气模型中以改进SOA大气负载、生命周期和影响预测的重要性。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Distinct Gas-Particle Partitioning and Viscosity Characteristics of Secondary Organic Aerosols Derived from α-Pinene versus Ocimene

Distinct Gas-Particle Partitioning and Viscosity Characteristics of Secondary Organic Aerosols Derived from α-Pinene versus Ocimene

Secondary organic aerosols (SOA) have complex, multicomponent composition that controls particle viscosity and gas-particle partitioning, key factors to their atmospheric evolution. This study investigates the chemical composition, volatility and viscosity of SOA formed by ozonolysis of cyclic α-pinene (PSOA) and acyclic ocimene (OSOA) monoterpenes. Using Temperature-Programmed Desorption combined with Direct Analysis in Real-Time ionization and High-Resolution Mass Spectrometry, we determined the molecular composition and saturation mass concentration of individual SOA constituents. These data enabled gas-particle partitioning and viscosity estimates under varied atmospheric conditions. PSOA, composed of higher molecular weight and less oxidized species, shows higher condensability and viscosity under high total organic mass (tOM) loadings. In contrast, OSOA, consisting of more oxidized, lower molecular weight species, exhibits greater sensitivity to tOM, with viscosity increasing significantly upon dilution. Poke-flow experiments support this trend, indicating that OSOA undergoes more dynamic compositional and phase changes during atmospheric aging. These observations reveal distinct dynamic trends in the atmospheric transformations and reactivity of SOA from cyclic and acyclic monoterpenes, with the latter showing greater compositional changes during aging that alter viscosity and diffusion. This highlights the importance of incorporating such dynamic transformations into atmospheric models to improve predictions of SOA atmospheric loadings, lifetimes, and impacts.

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