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首页> 外文期刊>Environmental Science & Technology >Particle Size Distribution Dynamics Can Help Constrain the Phase State of Secondary Organic Aerosol
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Particle Size Distribution Dynamics Can Help Constrain the Phase State of Secondary Organic Aerosol

机译：粒度分布动态可以有助于约束二次有机气溶胶的相位状态

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摘要

Particle phase state is a property of atmospheric aerosols that has important implications for the formation, evolution, and gas/particle partitioning of secondary organic aerosol (SOA). In this work, we use a size-resolved chemistry and microphysics model (Statistical Oxidation Model coupled to the TwO Moment Aerosol Sectional (SOM-TOMAS)), updated to include an explicit treatment of particle phase state, to constrain the bulk diffusion coefficient (D_b) of SOA produced from α-pinene ozonolysis. By leveraging data from laboratory experiments performed in the absence of a seed and under dry conditions, we find that the D_b for SOA can be constrained ((1-7) ×10~(-15) cm~2 s~(-1) in these experiments) by simultaneously reproducing the time-varying SOA mass concentrations and the evolution of the particle size distribution. Another version of our model that used the predicted SOA composition to calculate the glass-transition temperature, viscosity, and, ultimately, D_b (～10~(-15) cm~2 s~(-1)) of the SOA was able to reproduce the mass and size distribution measurements when we included oligomer formation (oligomers accounted for about a fifth of the SOA mass). Our work highlights the potential of a size-resolved SOA model to constrain the particle phase state of SOA using historical measurements of the evolution of the particle size distribution.
机译：粒子相位是大气气溶胶的性质，对二次有机气溶胶（SOA）的形成，进化和气体/颗粒分配具有重要意义。在这项工作中，我们使用尺寸分辨的化学和微物理模型（统计氧化模型，耦合到两时刻气溶胶截面（Som-Tomas）），更新以包括对粒子相位状态的显式治疗，以限制散装扩散系数（由α-脊烯臭氧溶解产生的SOA的D_B。通过在没有种子和干燥条件下在没有种子和干燥条件下进行的实验室实验中利用数据，我们发现SOA的D_B可以受约束（（1-7）×10〜（-15）cm〜2 s〜（-1）在这些实验中，通过同时再现时变的SOA质量浓度和粒度分布的演变。我们使用预测的SOA组合物来计算玻璃化转变温度，粘度和最终的模型的另一个版本，并且最终是SOA的D_B（〜10〜（-15）cm〜2 s〜（-1））当我们包括低聚物形成时再现质量和尺寸分布测量（低聚物占SOA质量的约5分）。我们的工作突出了尺寸分辨的SOA模型的潜力，以利用粒度分布的演化的历史测量来限制SOA的粒子相位状态。

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  • 来源
    《Environmental Science & Technology》 |2021年第3期|1466-1476|共11页
  • 作者

    Yicong He; Ali Akherati; Theodora Nah; Nga L. Ng; Lauren A. Garofalo; Delphine K. Farmer; Manabu Shiraiwa; Rahul A. Zaveri; Christopher D. Cappa; Jeffrey R. Pierce; Shantanu H. Jathar;

  • 作者单位

    Department of Mechanical Engineering Colorado State University Fort Collins Colorado 80523 United States;

    Department of Mechanical Engineering Colorado State University Fort Collins Colorado 80523 United States;

    School of Energy and Environment and State Key Laboratory of Marine Pollution City University of Hong Kong Hong Kong China;

    School of Chemical and Biomolecular Engineering Georgia Institute of Technology Atlanta Georgia 30332 United States School of Earth and Atmospheric Sciences and School of Civil and Environmental Engineering Georgia Institute of Technology Atlanta Georgia 30332 United States;

    Department of Chemistry Colorado State University Fort Collins Colorado 80523 United States;

    Department of Chemistry Colorado State University Fort Collins Colorado 80523 United States;

    Department of Chemistry University of California Irvine Irvine California 92697 United States;

    Sciences and Global Change Division Pacific Northwest National Laboratory Richland Washington 99354 United States;

    Department of Civil and Environmental Engineering University of California Davis Davis California 95616 United States;

    Department of Atmospheric Science Colorado State University Fort Collins Colorado 80523 United States;

    Department of Mechanical Engineering Colorado State University Fort Collins Colorado 80523 United States;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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