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夜间人为源-生物源相互作用:β-蒎烯氧化增强二次气溶胶和含氮、硫的颗粒有机物的形成。

Anthropogenic-Biogenic Interactions at Night: Enhanced Formation of Secondary Aerosols and Particulate Nitrogen- and Sulfur-Containing Organics from β-Pinene Oxidation.

机构信息

Environment Research Institute, Shandong University, Qingdao 266237, China.

Université Lyon, Université Claude Bernard Lyon 1, CNRS, IRCELYON, F-69626 Villeurbanne, France.

出版信息

Environ Sci Technol. 2021 Jun 15;55(12):7794-7807. doi: 10.1021/acs.est.0c07879. Epub 2021 May 27.

Abstract

Mixing of anthropogenic gaseous pollutants and biogenic volatile organic compounds impacts the formation of secondary aerosols, but still in an unclear manner. The present study explores secondary aerosol formation via the interactions between β-pinene, O, NO, SO, and NH under dark conditions. Results showed that aerosol yield can be largely enhanced by more than 330% by NO or SO but slightly enhanced by NH by 39% when the ratio of inorganic gases to β-pinene ranged from 0 to 1.3. Joint effects of NO and SO and SO and NH existed as aerosol yields increased with NO but decreased with NH when SO was kept constant. Infrared spectra showed nitrogen-containing aerosol components derived from NO and NH and sulfur-containing species derived from SO. Several particulate organic nitrates (MW 215, 229, 231, 245), organosulfates (MW 250, 264, 280, 282, 284), and nitrooxy organosulfates (MW 295, 311, 325, 327, and 343) were identified using high-resolution orbitrap mass spectrometry in NO and SO experiments, and their formation mechanism is discussed. Most of these nitrogen- and sulfur-containing species have been reported in ambient particles. Our results suggest that the complex interactions among β-pinene, O, NO, SO, and NH during the night might serve as a potential pathway for the formation of particulate nitrogen- and sulfur-containing organics, especially in polluted regions with both anthropogenic and biogenic influences.

摘要

人为气态污染物和生物挥发性有机化合物的混合会影响二次气溶胶的形成,但目前仍不清楚其具体影响方式。本研究探索了β-蒎烯、O、NO、SO 和 NH 在黑暗条件下相互作用形成二次气溶胶的过程。结果表明,当无机气体与β-蒎烯的比例在 0 到 1.3 之间时,NO 或 SO 可使气溶胶产率分别大幅提高 330%以上和 39%,而 NH 仅略微提高 39%。NO 和 SO 以及 SO 和 NH 的联合作用存在,当 SO 保持不变时,气溶胶产率随 NO 的增加而增加,随 NH 的增加而减少。红外光谱显示,NO 和 NH 产生含氮气溶胶成分,SO 产生含硫物质。利用高分辨轨道阱质谱在 NO 和 SO 实验中鉴定出几种颗粒态有机硝酸盐(MW 215、229、231、245)、有机硫酸盐(MW 250、264、280、282、284)和硝基氧有机硫酸盐(MW 295、311、325、327 和 343),并讨论了它们的形成机制。这些含氮和含硫的物质大多数已在环境颗粒中报道过。我们的结果表明,夜间β-蒎烯、O、NO、SO 和 NH 之间的复杂相互作用可能是形成颗粒态含氮和含硫有机化合物的潜在途径,尤其是在受到人为和生物源影响的污染地区。

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