溶解硫酸铵颗粒上乙二醛多相反应的在线形态研究

IF 2.9 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
Nicolas Brun*, Anil Kumar Mandariya, Junteng Wu, Francesco Battaglia, Jian Xu, Manon Rocco, Laurent Poulain, Mathieu Cazaunau, Antonin Berge, Edouard Pangui, Brice Temime-Roussel, Bénédicte Picquet-Varrault, Jean-Louis Clément, Aline Gratien, Paola Formenti, Liang Wen, Thomas Schaefer, Andreas Tilgner, Hartmut Herrmann, Jean-François Doussin and Anne Monod*, 
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引用次数: 0

摘要

在散装硫酸铵(AS)水溶液中,乙二醛和氨的反应在酸性条件下是缓慢的,这限制了它在潮湿的酸性气溶胶条件下的大气相关性。然而,先前的室内实验观察到在几分钟内气态乙二醛在硫酸铵颗粒上的反应性摄取过程中形成发色团。由于缺乏有机物种形成和相对湿度(RH)不允许种子颗粒潮解,其机制仍未得到解决。本文研究了在CESAM模拟室内,溶解的AS种子颗粒(相对湿度≥80±3%)吸收气态乙二醛时气体和颗粒相的化学形态。粒子的化学形态是使用AMS测量和CHARON-PTR-ToF-MS进行的。探讨了H2O2添加量、种子酸度和紫外-可见光解作用的影响。在所有实验中都一致观察到气体乙二醛在AS颗粒上的快速反应性吸收。两台质谱仪的联合测量结果通过对AMS数据进行正矩阵分解,实现了源解析分析,并鉴定和量化了三个主要过程:(i)乙二醛水化,(ii)乙二醛的快速暗老化,包括棕色碳的形成和(iii)光化学老化。CHARON-PTR-ToF-MS可以在室内实验中在几分钟内识别出个别产品,如恶唑和咪唑-2-甲醛。提出了乙二醛摄取的详细机制,强调了动力学和主要反应途径与散装水相中乙二醛反应活性的显着差异。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Online Speciation of Glyoxal Multiphase Reactions on Deliquesced Ammonium Sulfate Particles

Online Speciation of Glyoxal Multiphase Reactions on Deliquesced Ammonium Sulfate Particles

The reaction between glyoxal and ammonia in bulk Ammonium Sulfate (AS) aqueous solutions is known to be slow under acidic conditions, limiting its atmospheric relevance in wet acidic aerosol conditions. However, previous chamber experiments observed the formation of chromophores during the reactive uptake of gaseous glyoxal on ammonium sulfate particles within minutes. The mechanisms remained unresolved due to the lack of organic speciation and the Relative Humidity (RH) did not allow the seed particles to deliquesce. This study presents chemical speciation of the gas and the particle phases during the uptake of gaseous glyoxal on deliquesced AS seed particles (RH ≥ 80 ± 3%) in the CESAM simulation chamber. The chemical speciation of the particles was performed using AMS measurements complemented by a CHARON-PTR-ToF-MS. The influence of H2O2 addition, seed acidity and UV–vis photolysis was explored. Fast reactive uptake of gaseous glyoxal on AS particles was consistently observed in all experiments. The combined measurements from the two mass spectrometers enabled source apportionment analysis through positive matrix factorization of the AMS data and led to the identification and quantification of three dominant processes: (i) glyoxal hydration, (ii) fast dark aging of glyoxal, including the formation of brown carbon and (iii) photochemical aging. The CHARON-PTR-ToF-MS allowed the identification of individual products, such as oxazole and imidazole-2-carboxaldehyde, appearing within minutes during the chamber experiments. A detailed mechanism of glyoxal uptake was proposed, highlighting significant differences in kinetics and dominant reaction pathways compared to the glyoxal reactivity in the bulk aqueous phase.

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来源期刊
ACS Earth and Space Chemistry
ACS Earth and Space Chemistry Earth and Planetary Sciences-Geochemistry and Petrology
CiteScore
5.30
自引率
11.80%
发文量
249
期刊介绍: The scope of ACS Earth and Space Chemistry includes the application of analytical, experimental and theoretical chemistry to investigate research questions relevant to the Earth and Space. The journal encompasses the highly interdisciplinary nature of research in this area, while emphasizing chemistry and chemical research tools as the unifying theme. The journal publishes broadly in the domains of high- and low-temperature geochemistry, atmospheric chemistry, marine chemistry, planetary chemistry, astrochemistry, and analytical geochemistry. ACS Earth and Space Chemistry publishes Articles, Letters, Reviews, and Features to provide flexible formats to readily communicate all aspects of research in these fields.
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