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Ionic Strength Effect on Photochemistry of Fluorene and Dimethylsulfoxide at the Air–Sea Interface: Alternative Formation Pathway of Organic Sulfur Compounds in a Marine Atmosphere
ACS Earth and Space Chemistry ( IF 2.9 ) Pub Date : 2020-06-01 , DOI: 10.1021/acsearthspacechem.0c00059
Majda Mekic 1, 2 , Jiafa Zeng 3 , Wentao Zhou 1, 2 , Gwendal Loisel 1 , Biao Jin 1 , Xue Li 3 , Davide Vione 4 , Sasho Gligorovski 1
Affiliation  

The photochemical transformation processes occurring at the sea surface lead to the formation of low volatility organic compounds that contribute to new particle formation in the marine boundary layer. Here, we suggest an alternative formation pathway of organosulfur and oxygenated aliphatic compounds, initiated by sunlight-activated fluorene (FL) and dimethylsulfoxide (DMSO) in the presence of the halide ions Cl, Br, and I. In particular, we observe a prompt formation of four typical precursors of secondary organic aerosols, methanesulfonic acid (CH3SO3H), methanesulfinic acid (CH3SO2H), hydroxymethanesulfonic acid (CH4O4S, MSAOH), and 2-hydroxyethenesulfonic acid (C2H5O4SH), upon light irradiation of FL/DMSO. The photochemical modeling shows that in the summer period, MSAOH would be formed in just a few hours under fair-weather conditions, which makes the photosensitized chemistry of FL toward DMSO potentially significant. We also show that the sunlight-initiated degradation of FL is considerably faster in the presence of halide ions, compared to its photochemical degradation in the dilute aqueous phase. Therefore, the photochemical degradation of FL and potentially other polycyclic aromatic hydrocarbons would be faster in high ionic strength aerosol particles, compared to analogous diluted aqueous-phase photochemical processes occurring in, for example, clouds. This could considerably affect the absorbing properties of the aerosols, which should be considered in future modeling studies.

中文翻译:

离子强度对海-气界面中芴和二甲基亚砜光化学的影响:海洋大气中有机硫化合物的替代形成途径

在海面发生的光化学转化过程导致形成低挥发性有机化合物,这些有机化合物有助于在海洋边界层中形成新的颗粒。在这里,我们建议的有机硫替代形成途径和氧化的脂族化合物,通过在卤化物存在日光活化的芴(FL)和二甲亚砜(DMSO)发起离子氯- ,溴-和I - 。特别是,我们观察到迅速形成了二次有机气溶胶的四种典型前体:甲磺酸(CH 3 SO 3 H),甲磺酸(CH 3 SO 2 H),羟基甲磺酸(CH 4 O)。4 S,MSAOH)和2-羟基乙烯磺酸(C 2 H 5 O 4SH),在FL / DMSO的光照射下。光化学模型表明,在夏季,在晴朗的天气条件下,仅需几个小时即可形成MSAOH,这使得FL对DMSO的光敏化学反应具有重要意义。我们还表明,与卤素在稀水相中的光化学降解相比,在卤离子存在下,阳光引发的FL降解要快得多。因此,与例如在云中发生的类似的稀释水相光化学过程相比,高离子强度气溶胶颗粒中FL和潜在的其他多环芳烃的光化学降解将更快。这可能会严重影响气溶胶的吸收特性,这在以后的建模研究中应予以考虑。
更新日期:2020-07-16
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