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

How salt lakes affect atmospheric new particle formation: A case study in Western Australia.
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盐湖如何影响大气新颗粒的形成:西澳大利亚的案例研究

DOI:
10.1016/j.scitotenv.2016.08.058
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发表时间:
2016
期刊:
The Science of the total environment
影响因子:
--
通讯作者:
Schöler
Schöler
中科院分区:
--
文献类型:
--
作者:
Kamilli;Krause;Sattler;Schmitt-Kopplin;Eitenberger;Friedbacher;Lohninger;Schöler

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在澳大利亚西部7个不同盐湖的盐壳和富有机质层上方,利用移动气溶胶室对盐湖上的新颗粒形成进行了原位研究。这种独特的设置使探索盐湖排放对大气新粒子形成的影响成为可能,并确定水相和气相化学的相互作用。新粒子的形成通常在气温升高和太阳辐照度增强的情况下观察到。挥发性有机化合物从盐湖表面释放出来,可能来自富含分解凋落叶的有机化合物的土层,并积聚在室内空气中。这些有机前驱体气体氧化后,反应产物形成了新的颗粒,其生长速率为2.7 ~ 25.4 nm h−1。在新颗粒形成事件发生之前,盐湖水中亚铁和三铁的存在以及pH值的下降表明有机化合物在水相中也被氧化,影响了大气中新颗粒的形成过程。假设水相化学对新粒子形成的贡献,因为数百种氧化有机化合物的混合物用几种分析技术进行了表征。这种化学成分多样化的有机气溶胶部分含有含硫和含氮的有机化合物,以及卤化有机化合物。采用电子显微镜、能量色散x射线光谱和拉曼光谱对粗模粒子进行了分析。采用超高分辨率质谱法对过滤后的样品进行分析。目标质谱分析揭示了单萜烯前体形成的有机硫酸盐和1,8-桉树脑大气氧化形成的二级有机气溶胶的两种已知示踪剂,这表明单萜烯的水相和气相氧化的复杂相互作用有助于在所研究的盐湖环境中形成新的颗粒。
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 25.4 nm h− 1. 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.
DOI: 10.1021/acs.analchem.5b02272
发表时间: 2015-09-15
影响因子: 7.4
作者:
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DOI: 10.5194/acp-12-5787-2012
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影响因子: 6.3
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DOI: 10.1021/es051294x
发表时间: 2006-02-15
影响因子: 11.4
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DOI: 10.1039/c3fd00093a
发表时间: 2013-12
影响因子: 3.4
作者:
J. Ofner;K. Kamilli;A. Held;B. Lendl;C. Zetzsch
通讯作者: J. Ofner;K. Kamilli;A. Held;B. Lendl;C. Zetzsch
DOI: 10.1002/kin.20714
发表时间: 2012
影响因子: 1.5
作者:
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通讯作者: C. Zetzsch