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Formation of Organosulfur Compounds through Transition Metal Ion-Catalyzed Aqueous Phase Reactions
Environmental Science & Technology Letters ( IF 10.9 ) Pub Date : 2018-05-25 , DOI: 10.1021/acs.estlett.8b00225
Liubin Huang 1 , Richard E. Cochran 1 , Ellen M. Coddens 1 , Vicki H. Grassian 1
Affiliation  

Organosulfur compounds, particularly organosulfates, are considered as important tracers of secondary organic aerosol formation. However, the mechanistic pathways for the formation of these compounds in the atmosphere are still not well understood. In this study, we show for the first time that C2–C4 organosulfur compounds, as well as their oligomers, can form in the aqueous phase from reactions of unsaturated carbonyl compounds, i.e., methacrolein (MACR) and methyl vinyl ketone (MVK), with the bisulfite anion (HSO3) in the presence of Fe3+. The mechanism for product formation in the presence of Fe3+ involves sulfite and sulfate ion radicals. As shown here, the formation of specific organosulfur compounds depends on the concentrations of MVK and MACR and the solution pH. Our findings provide new insights into pathways for forming organosulfur compounds in the atmosphere and the role that transition metal ions, such as Fe3+, play in catalyzing these reactions.

中文翻译:

通过过渡金属离子催化的水相反应形成有机硫化合物

有机硫化合物,特别是有机硫酸盐,被认为是二次有机气溶胶形成的重要示踪剂。但是,对于在大气中形成这些化合物的机制途径仍然知之甚少。在这项研究中,我们首次表明,C 2 –C 4有机硫化合物及其低聚物可以从不饱和羰基化合物(即甲基丙烯醛(MACR)和甲基乙烯基酮(MVK))的反应中形成于水相中。 ),以及在亚铁3+存在下与亚硫酸氢根阴离子(HSO 3 )。Fe 3+存在下产物形成的机理涉及亚硫酸根和硫酸根离子自由基。如此处所示,特定有机硫化合物的形成取决于MVK和MACR的浓度以及溶液的pH值。我们的发现为在大气中形成有机硫化合物的途径以及过渡金属离子(例如Fe 3+)在催化这些反应中的作用提供了新见解。
更新日期:2018-05-27
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