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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：区域规模的拉格朗日田野试验所约束的海洋大气中硝基PAHs的快速形成

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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（PAH）及其某些硝化衍生物NPAH在大气环境中似乎无处不在。但是，大气寿命可能会在很宽的范围内变化，并且可能短至几个小时。大气中NPAH的来源和吸收尚不清楚。通过拉格朗日野外实验和建模，我们在无云的海洋环境中研究了半挥发性PAHs荧蒽和pyr在无云的海洋大气中转化为2-硝基衍生物2-硝基荧蒽和2-硝基py的时间，时间范围为1小时到1天之间。沿海和岛屿站点。通过拉格朗日盒模型（即与拉格朗日粒子分散模型FLEXPART-WRF耦合的盒模型）模拟了几次发作期间的化学和运输。发现化学动力学数据确实捕获了在环境条件下数小时至1天的时间范围内4环PAHs的光化学降解，同时产生了相应的NPAH，该NPAH维持了2-硝基荧蒽/荧蒽和2-硝基py py的产率分别被低估了（3.7 +/- 0.2）％和（1.5 +/- 0.1）％。当通过理论上的估计来探索描述OH加合物反应性的动力学数据时，预测的NPAH水平接近观察到的水平。当采用在高NOx条件下进行的实验室实验报告的NPAH / PAH产量进行模拟时，预测值也会低估1-2个数量级。结论是，在低NOx条件下有效的NPAH来源被大大低估了。

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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;

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