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Photosensitized Degradation of DMSO Initiated by PAHs at the Air-Water Interface, as an Alternative Source of Organic Sulfur Compounds to the Atmosphere

机译:多环芳烃在空气-水界面引发的DMSO光敏降解,作为有机硫化合物进入大气的替代来源

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摘要

The photochemical reactions of organic compounds at the water surface lead to the formation of gas-phase molecules that may contribute to new particle formation in the atmosphere. Here, we observe the formation of organic sulfur (OS) compounds that are known secondary organic aerosol (SOA) precursors, upon irradiation of aqueous solutions containing typical polycyclic aromatic hydrocarbons (PAHs) such as pyrene, fluoranthene, and phenanthrene as well as dimethylsulfoxide (DMSO). The reactivity between the excited triplet states of PAHs ((3)PAHs*) and DMSO was determined by transient absorption spectroscopy and a tentative reaction mechanism for DMSO degradation was proposed, supported by theoretical calculations of the reaction Gibbs energies. In all cases, we observe rapid formation of methanesulfonic acid, methanesulfinic acid, methylsulfonylmethane, ethyl methanesulfonate, hydroxymethanesulfonic acid, and 2-hydroxyethanesulfonic acid by use of novel membrane inlet-single photon ionization-time of flight mass spectrometry. These results suggest that ubiquitous PAHs and DMSO at the sea surface may represent an alternative source of OS compounds during daytime, through photochemical processes that should be considered in future models to better represent the SOA formation processes in the atmosphere.
机译:有机化合物在水面上的光化学反应导致气相分子的形成,这可能有助于在大气中形成新的颗粒。在这里,我们观察到有机硫 (OS) 化合物的形成,这些化合物是已知的次级有机气溶胶 (SOA) 前体,在辐照含有典型多环芳烃 (PAH) 的水溶液(如芘、荧蒽和菲)以及二甲基亚砜 (DMSO)。通过瞬态吸收光谱测定了PAHs((3)PAHs*)激发三重态与DMSO之间的反应活性,并结合反应吉布斯能量的理论计算,提出了DMSO降解的试探性反应机理。在所有情况下,我们通过使用新型膜入口-单光子电离-飞行时间质谱法观察到甲磺酸、甲亚磺酸、甲基磺酰甲烷、甲磺酸乙酯、羟基甲磺酸和 2-羟基乙磺酸的快速形成。这些结果表明,海面上无处不在的多环芳烃和DMSO可能代表了白天OS化合物的替代来源,通过光化学过程,在未来的模型中应考虑这些过程,以更好地代表大气中SOA的形成过程。

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