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首页> 外文期刊>Environmental Science & Technology >Fast Formation of Nitro-PAHs in the Marine Atmosphere Constrained in a Regional-Scale Lagrangian Field Experiment
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Fast Formation of Nitro-PAHs in the Marine Atmosphere Constrained in a Regional-Scale Lagrangian Field Experiment

机译：在海洋气氛中快速形成硝基-PAH在区域级拉格朗日实践中受到约束

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摘要

Polycyclic aromatic hydrocarbons (PAHs) and some of their nitrated derivatives, NPAHs, are seemingly ubiquitous in the atmospheric environment. Atmospheric lifetimes may nevertheless vary within a wide range, and be as short as a few hours. The sources and sinks of NPAH in the atmosphere are not well understood. With a Lagrangian field experiment and modeling, we studied the conversion of the semivolatile PAHs fluoranthene and pyrene into the 2-nitro derivatives 2-nitrofluoranthene and 2-nitropyrene in a cloud-free marine atmosphere on the time scale of hours to 1 day between a coastal and an island site. Chemistry and transport during several episodes was simulated by a Lagrangian box model i.e., a box model coupled to a Lagrangian particle dispersion model, FLEXPART-WRF. It is found that the chemical kinetic data do capture photochemical degradation of the 4-ring PAHs under ambient conditions on the time scale of hours to 1 day, while the production of the corresponding NPAH, which sustained 2-nitrofluoranthene/fluoranthene and 2-nitropyrene/pyrene yields of (3.7 +/- 0.2) and (1.5 +/- 0.1)%, respectively, is by far underestimated. Predicted levels of NPAH come close to observed ones, when kinetic data describing the reactivity of the OH-adduct were explored by means of theoretically based estimates. Predictions are also underestimated by 1-2 orders of magnitude, when NPAH/PAH yields reported from laboratory experiments conducted under high NOx conditions are adopted for the simulations. It is concluded that NPAH sources effective under low NOx conditions, are largely underestimated.
机译：多环芳烃（PAHS）和一些硝化衍生物NPAH在大气环境中看似普遍存在。迄今为止，大气寿命可能在宽范围内变化，并且短短几个小时。在大气中NPAH的来源和汇不会很好地理解。通过拉格朗日野外实验和建模，我们将半抗菌性PAHS氟和芘转化为2-硝基衍生物2-硝基氟苯和2-硝基在无云海洋气氛中，在一个小时至1天之间的时间等级沿海和岛屿网站。通过拉格朗日盒模型，耦合到拉格朗日粒子分散模型，FlexPart-WRF的盒子模型，将化学和运输进行了模拟。结果发现化学动力学数据确实在每小时到1天的时间范围内捕获4环PAHs的光化学降解，而相应的NPAH的产生，其持续2-氮氟蒽/氟和2-硝基乙烯/芘产率分别为（3.7 +/- 0.2）和（1.5 +/- 0.1）％，是远定估计的。当通过理论基于基于估计探索了描述OH-加合物的反应性的动力学数据，预测的NPAH的水平接近观察到的。当采用在高NOx条件下进行的实验室实验报告的NPAH / PAH产量被用于模拟时，预测也低估了1-2级数量级。结论是，在低NOx条件下有效的NPAH源主要低估。

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  • 来源
    《Environmental Science & Technology》 |2019年第15期|8914-8924|共11页
  • 作者

    Mulder Marie D.; Dumanoglu Yetkin; Efstathiou Christos; Kukucka Petr; Matejovicova Jana; Maurer Christian; Pribylova Petra; Prokes Roman; Sofuoglu Aysun; Sofuoglu Sait C.; Wilson Jake; Zetzsch Cornelius; Wotawa Gerhard; Lammel Gerhard;

  • 作者单位

    Masaryk Univ Res Ctr Tox Cpds Environm Kamenice 5 Brno 62500 Czech Republic|Zentralanstalt Meteorol & Geodynam Vienna Austria;

    Dokuz Eylul Univ Environm Engn Dept Izmir Turkey;

    Masaryk Univ Res Ctr Tox Cpds Environm Kamenice 5 Brno 62500 Czech Republic;

    Masaryk Univ Res Ctr Tox Cpds Environm Kamenice 5 Brno 62500 Czech Republic;

    Masaryk Univ Res Ctr Tox Cpds Environm Kamenice 5 Brno 62500 Czech Republic|Slovak Hydrometeorol Inst Bratislava Slovakia;

    Zentralanstalt Meteorol & Geodynam Vienna Austria;

    Masaryk Univ Res Ctr Tox Cpds Environm Kamenice 5 Brno 62500 Czech Republic;

    Masaryk Univ Res Ctr Tox Cpds Environm Kamenice 5 Brno 62500 Czech Republic;

    Izmir Inst Technol Chem Engn Dept Urla Turkey;

    Izmir Inst Technol Chem Engn Dept Urla Turkey|Izmir Inst Technol Environm Engn Dept Urla Turkey;

    Max Planck Inst Chem Multiphase Chem Dept Mainz Germany;

    Max Planck Inst Chem Multiphase Chem Dept Mainz Germany;

    Zentralanstalt Meteorol & Geodynam Vienna Austria;

    Masaryk Univ Res Ctr Tox Cpds Environm Kamenice 5 Brno 62500 Czech Republic|Max Planck Inst Chem Multiphase Chem Dept Mainz Germany;

  • 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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