New particle formation above a simulated salt lake in aerosol chamber experiments

New particle formation above a simulated salt lake in aerosol chamber experiments
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气溶胶室实验中模拟盐湖上方新颗粒的形成

DOI:
10.1071/en14225
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发表时间:
2015
影响因子:
4.3
通讯作者:
Schmitt-Kopplin
Schmitt-Kopplin
中科院分区:
环境科学与生态学4区
文献类型:
--
作者:
Kamilli;Schmitt-Kopplin

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环境背景西澳大利亚州从世纪中期开始的森林砍伐导致了土地表面的巨大变化,西澳大利亚州现在更经常遭受干旱。由盐湖引起的颗粒形成已被确定为改变降水模式的潜在控制因素。本研究的目的是通过在实验室气溶胶室内模拟一个简化的盐湖来确定颗粒形成过程中的关键因素。摘要在最近的野外实验中,在西澳大利亚的盐湖上方观察到了颗粒的形成,并与区域降水模式的变化有关。本文研究了在不同条件下,模拟盐湖气溶胶室实验中颗粒形成的可能性。该盐湖混合物包括固定浓度的NaBr、NaCl和Na 2SO 4,以及不同浓度的FeSO 4和FeCl 3。此外,在黑暗和光照条件下加入1,8-桉叶醇和柠檬烯的有机混合物。在我们的实验中,发现有机化合物和光的存在对于新粒子的形成都是必不可少的。有明确的迹象表明,Fe II到Fe III的转换,这表明在系统中的芬顿反应机制。相反的想法,一个芬顿样的反应机制可能会加剧有机物的氧化,从而促进二次有机气溶胶的形成,所观察到的颗粒形成开始较晚,并具有较低的强度下升高的Fe II浓度。当从实验中排除Fe II时,观察到最高的颗粒数浓度。形成的气溶胶的化学分析证实了在这项研究中的粒子形成的芬顿反应的重要作用。超高分辨率质谱和拉曼光谱提供了分析证据的有机硫酸盐和卤代有机化合物在实验中提出的形成。尽管卤素和有机前体在这些实验模拟中是丰富的,卤素诱导的有机气溶胶形成的存在,但似乎在颗粒形成中起着次要的整体作用。
Environmental context Deforestation in Western Australia beginning in the mid-19th century led to a considerable change of the land surface, and Western Australia is now suffering more often from droughts. Particle formation induced by salt lakes has been identified as a potential control factor for changed precipitation patterns. This study aims to determine key factors involved in the particle formation process by simulating a simplified salt lake in an aerosol chamber in the laboratory. Abstract In recent field experiments, particle formation has been observed above salt lakes in Western Australia and related to changes in regional precipitation patterns. This work investigates the particle formation potential above a simulated salt lake in aerosol chamber experiments under various conditions. The salt lake mixture comprised fixed concentrations of NaBr, NaCl and Na2SO4, and varying concentrations of FeSO4 and FeCl3. Further, an organic mixture of 1,8-cineol and limonene was added under dark and light conditions. Both the presence of organic compounds and of light were found to be essential for new particle formation in our experiments. There were clear indications for conversion of FeII to FeIII, which suggests a Fenton-like reaction mechanism in the system. Contrary to the idea that a Fenton-like reaction mechanism might intensify the oxidation of organic matter, thus facilitating secondary organic aerosol formation, the observed particle formation started later and with lower intensity under elevated FeII concentrations. The highest particle number concentrations were observed when excluding FeII from the experiments. Chemical analysis of the formed aerosol confirmed the important role of the Fenton-like reaction for particle formation in this study. Ultrahigh-resolution mass spectrometry and Raman spectroscopy provide analytical proof for the formation of organosulfates and halogenated organic compounds in the experiments presented. Even though halogens and organic precursors are abundant in these experimental simulations, halogen-induced organic aerosol formation exists but seems to play a minor overall role in particle formation.
DOI: 10.1021/es051294x
发表时间: 2006-02-15
影响因子: 11.4
作者:
Batonneau, Y;Sobanska, S;Bremard, C
通讯作者: Bremard, C
DOI: 10.1039/c3fd00093a
发表时间: 2013-12
影响因子: 3.4
作者:
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DOI: 10.1021/es00175a004
发表时间: 1988-10-01
影响因子: 11.4
作者:
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DOI: 10.5194/acp-11-1-2011
发表时间: 2011-01-01
影响因子: 6.3
作者:
Ofner, J.;Krueger, H. -U.;Zetzsch, C.
通讯作者: Zetzsch, C.
DOI: 10.1021/es00080a007
发表时间: 1990-10-01
影响因子: 11.4
作者:
CORCHNOY, SB;ATKINSON, R
通讯作者: ATKINSON, R