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首页> 外文期刊>Environmental Science & Technology >Reactive Uptake of an Isoprene-Derived Epoxydiol to Submicron Aerosol Particles
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Reactive Uptake of an Isoprene-Derived Epoxydiol to Submicron Aerosol Particles

机译:异戊二烯衍生的环氧二醇对亚微米气溶胶颗粒的反应性吸收

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摘要

The reactive uptake of isoprene-derived epoxydiols (IEPOX) is thought to be a significant source of atmospheric secondary organic aerosol (SOA). However, the IEPOX reaction probability (γ_(IEPOX)) and its dependence upon particle composition remain poorly constrained. We report measurements of γ_(IEPOX) for trans-β-IEPOX, the predominant IEPOX isomer, on submicron particles as a function of composition, acidity, and relative humidity (RH). Particle acidity had the strongest effect. γ_(IEPOX) is more than 500 times greater on ammonium bisulfate (γ ~ 0.05) than on ammonium sulfate (γ ≤ 1 × 10~(-4)). We could accurately predict γ_(IEPOX) using an acid-catalyzed, epoxide ring-opening mechanism and a high Henry's law coeiEcient (1.7 × 10~8 M/ atm). Suppression of γ_(IEPOX) was observed on particles containing both ammonium bisulfate and poly(ethylene glycol) (PEG-300), likely due to diffusion and solubility limitations within a PEG-300 coating, suggesting that IEPOX uptake could be self-limiting. Using the measured uptake kinetics, the predicted atmospheric lifetime of IEPOX is a few hours in the presence of highly acidic particles (pH < 0) but is greater than 25 h on less acidic particles (pH > 3). This work highlights the importance of aerosol acidity for accurately predicting the fate of IEPOX and anthropogenically influenced biogenic SOA formation.
机译:异戊二烯衍生的环氧二醇(IEPOX)的反应性吸收被认为是大气次级有机气溶胶(SOA)的重要来源。但是,IEPOX反应概率(γ_(IEPOX))及其对颗粒组成的依赖性仍然受到约束。我们报告了对亚微米颗粒上反式-β-IEPOX(主要的IEPOX异构体)的γ_(IEPOX)的测量,该测量是成分,酸度和相对湿度(RH)的函数。颗粒酸度影响最大。硫酸氢铵(γ〜0.05)的γ_(IEPOX)比硫酸铵(γ≤1×10〜(-4))大500倍以上。我们可以使用酸催化的环氧化物开环机制和高亨利定律系数(1.7×10〜8 M / atm)准确地预测γ_(IEPOX)。在同时包含硫酸氢铵和聚乙二醇(PEG-300)的颗粒上观察到γ_(IEPOX)的抑制,这可能是由于PEG-300涂层内的扩散和溶解度限制所致,这表明IEPOX的吸收可能是自限性的。使用测得的吸收动力学,在高酸性颗粒(pH <0)存在下,IEPOX的预测大气寿命为数小时,而在弱酸性颗粒(pH> 3)下,IEPOX的预期大气寿命大于25小时。这项工作强调了气溶胶酸度对于准确预测IEPOX的命运和人为影响的生物SOA形成的重要性。

著录项

  • 来源
    《Environmental Science & Technology》 |2014年第19期|11178-11186|共9页
  • 作者单位

    Department of Atmospheric Sciences, University of Washington, Seattle, Washington 98195 United States;

    Department of Environmental Sciences and Engineering, Gillings School of Global Public Health, University of North Carolina, Chapel Hill, North Carolina 27599 United States;

    Department of Environmental Sciences and Engineering, Gillings School of Global Public Health, University of North Carolina, Chapel Hill, North Carolina 27599 United States;

    Department of Environmental Sciences and Engineering, Gillings School of Global Public Health, University of North Carolina, Chapel Hill, North Carolina 27599 United States;

    Department of Environmental Sciences and Engineering, Gillings School of Global Public Health, University of North Carolina, Chapel Hill, North Carolina 27599 United States;

    Department of Atmospheric Sciences, University of Washington, Seattle, Washington 98195 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);
  • 原文格式 PDF
  • 正文语种 eng
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