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Hygroscopic behavior of multicomponent organic aerosols and their internal mixtures with ammonium sulfate

机译:硫酸铵的多组分有机气溶胶及其内部混合物的吸湿性

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摘要

Water-soluble organic compounds (WSOCs) are important components of organics in the atmospheric fine particulate matter. Although WSOCs play an important role in the hygroscopicity of aerosols, knowledge on the water uptake behavior of internally mixed WSOC aerosols remains limited. Here, the hygroscopic properties of single components such as levoglucosan, oxalic acid, malonic acid, succinic acid, phthalic acid, and multicomponent WSOC aerosols mainly involving oxalic acid are investigated with the hygroscopicity tandem differential mobility analyzer (HTDMA). The coexisting hygroscopic species including levoglucosan, malonic acid, and phthalic acid have a strong influence on the hygroscopic growth and phase behavior of oxalic acid, even suppressing its crystallization completely during the drying process. The phase behaviors of oxalic acid/levoglucosan mixed particles are confirmed by infrared spectra. The discrepancies between measured growth factors and predictions from Extended Aerosol Inorganics Model (E-AIM) with the Universal Quasi-Chemical Functional Group Activity Coefficient (UNIFAC) method and Zdanovskii-Stokes-Robinson (ZSR) approach increase at medium and high relative humidity (RH) assuming oxalic acid in a crystalline solid state. For the internal mixture of oxalic acid with levoglucosan or succinic acid, there is enhanced water uptake at high RH compared to the model predictions based on reasonable oxalic acid phase assumption. Organic mixture has more complex effects on the hygroscopicity of ammonium sulfate than single species. Although hygroscopic species such as levoglucosan account for a small fraction in the multicomponent aerosols, they may still strongly influence the hygroscopic behavior of ammonium sulfate by changing the phase state of oxalic acid which plays the role of 'intermediate' species. Considering the abundance of oxalic acid in the atmospheric aerosols, its mixtures with hygroscopic species may significantly promote water uptake under high RH conditions and thus affect the cloud condensation nuclei (CCN) activity, optical properties, and chemical reactivity of atmospheric particles.
机译:水溶性有机化合物(WSOCS)是大气细颗粒物有机物的重要组成部分。虽然WSOCS在气溶胶吸湿性中发挥着重要作用,但是关于内部混合的WSOC气溶胶的水吸收行为的知识仍然有限。这里,用湿润程度串联差分迁移率分析仪(HTDMA)研究了主要涉及草酸的单一组分如左葡聚糖,草酸,丙二酸,琥珀酸,邻苯二甲酸和多组分WSOC气溶胶的吸湿性。包括左葡聚糖,丙酸和邻苯二甲酸在内的共存吸湿物种对草酸的吸湿生长和相行为产生强烈影响,甚至在干燥过程中完全抑制其结晶。草酸/左葡葡聚糖混合颗粒的相行为通过红外光谱证实。测量的生长因子与延长气溶胶无机模型(E-AIM)的预测与通用准化学官能团活动系数(UNIFAC)方法和Zdanovskii-Stokes-Robinson(ZSR)方法在中等和高相对湿度下增加( RH)假设在结晶固态中的草酸。对于具有左葡萄糖或琥珀酸的草酸的内部混合物,与基于合理的草酸相位假设的模型预测相比,高RH的水摄取增强。有机混合物对硫酸铵的吸湿性具有比单一物种更复杂的效果。虽然左葡聚糖如左葡聚糖如左葡聚糖的吸湿物种占多组分气溶胶中的一小部分,但它们仍然可能通过改变发挥“中间体”作用的草酸的相位态来强烈影响硫酸铵的吸湿性行为。考虑到大气气溶胶中的草酸丰度,其具有吸湿性物质的混合物可以显着促进高Rh条件下的水吸收,从而影响云缩小核(CCN)活性,光学性质和大气颗粒的化学反应性。

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  • 来源
    《Atmospheric chemistry and physics》 |2016年第6期|共18页
  • 作者单位

    Chinese Acad Sci Inst Chem State Key Lab Struct Chem Unstable &

    Stable Speci Beijing Natl Lab Mol Sci Beijing 100190 Peoples R China;

    Chinese Acad Sci Inst Chem State Key Lab Struct Chem Unstable &

    Stable Speci Beijing Natl Lab Mol Sci Beijing 100190 Peoples R China;

    Chinese Acad Sci Inst Chem State Key Lab Struct Chem Unstable &

    Stable Speci Beijing Natl Lab Mol Sci Beijing 100190 Peoples R China;

    Chinese Acad Sci Inst Chem State Key Lab Struct Chem Unstable &

    Stable Speci Beijing Natl Lab Mol Sci Beijing 100190 Peoples R China;

    Chinese Acad Sci Inst Chem State Key Lab Struct Chem Unstable &

    Stable Speci Beijing Natl Lab Mol Sci Beijing 100190 Peoples R China;

    Beijing Inst Technol Inst Chem Phys Sch Chem Beijing 100081 Peoples R China;

    Chinese Acad Sci Inst Chem State Key Lab Struct Chem Unstable &

    Stable Speci Beijing Natl Lab Mol Sci Beijing 100190 Peoples R China;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 大气科学(气象学);
  • 关键词

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