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盐湖如何影响大气中新粒子的形成:以澳大利亚西部为例。

How salt lakes affect atmospheric new particle formation: A case study in Western Australia.

机构信息

Atmospheric Chemistry, University of Bayreuth, Bayreuth, Germany.

Institute of Chemical Technologies and Analytics, TU Wien, Vienna, Austria.

出版信息

Sci Total Environ. 2016 Dec 15;573:985-995. doi: 10.1016/j.scitotenv.2016.08.058. Epub 2016 Sep 4.

Abstract

New particle formation was studied above salt lakes in-situ using a mobile aerosol chamber set up above the salt crust and organic-enriched layers of seven different salt lakes in Western Australia. This unique setup made it possible to explore the influence of salt lake emissions on atmospheric new particle formation, and to identify interactions of aqueous-phase and gas-phase chemistry. New particle formation was typically observed at enhanced air temperatures and enhanced solar irradiance. Volatile organic compounds were released from the salt lake surfaces, probably from a soil layer enriched in organic compounds from decomposed leaf litter, and accumulated in the chamber air. After oxidation of these organic precursor gases, the reaction products contributed to new particle formation with observed growth rates from 2.7 to 25.4nmh. The presence of ferrous and ferric iron and a drop of pH values in the salt lake water just before new particle formation events indicated that organic compounds were also oxidized in the aqueous phase, affecting the new particle formation process in the atmosphere. The contribution of aqueous-phase chemistry to new particle formation is assumed, as a mixture of hundreds of oxidized organic compounds was characterized with several analytical techniques. This chemically diverse composition of the organic aerosol fraction contained sulfur- and nitrogen-containing organic compounds, and halogenated organic compounds. Coarse mode particles were analyzed using electron microscopy, energy dispersive X-ray spectroscopy and Raman spectroscopy. Ultra-high resolution mass spectrometry was applied to analyze filter samples. A targeted mass spectral analysis revealed the formation of organosulfates from monoterpene precursors and two known tracers for secondary organic aerosol formation from atmospheric oxidation of 1,8-cineole, which indicates that a complex interplay of aqueous-phase and gas-phase oxidation of monoterpenes contributes to new particle formation in the investigated salt lake environment.

摘要

利用安装在盐壳和西澳大利亚七个不同盐湖富含有机物层上方的移动气溶胶室,对盐湖上的新粒子形成进行了现场研究。这种独特的设置使我们能够探索盐湖排放对大气中新粒子形成的影响,并确定水相和气相间化学相互作用。通常在空气温度升高和太阳辐射增强的情况下观察到新粒子形成。挥发性有机化合物从盐湖表面释放出来,可能是从富含分解落叶有机化合物的土壤层中释放出来的,并在腔室内空气中积累。这些有机前体气体氧化后,反应产物有助于新粒子形成,观察到的生长速率为 2.7 至 25.4nmh。在新粒子形成事件之前,盐湖水中亚铁和三价铁的存在以及 pH 值的下降表明,有机化合物也在水相中被氧化,这影响了大气中新粒子形成过程。假设水相化学对新粒子形成有贡献,因为使用几种分析技术对数百种氧化有机化合物的混合物进行了表征。有机气溶胶部分的这种化学组成多样,包含含硫和含氮有机化合物以及卤代有机化合物。使用电子显微镜、能量色散 X 射线光谱和拉曼光谱对粗模态颗粒进行了分析。超高效分辨率质谱仪用于分析滤膜样品。有针对性的质谱分析表明,单萜前体形成了有机硫酸盐,1,8-桉树脑大气氧化形成了两种已知的二次有机气溶胶形成示踪剂,这表明单萜在水相和气相间的复杂相互作用有助于研究盐湖环境中的新粒子形成。

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