Atmospheric Environment ( IF 5 ) Pub Date : 2021-04-29 , DOI: 10.1016/j.atmosenv.2020.118148 Paul Van Rooy , Kathleen L. Purvis-Roberts , Philip J. Silva , Matthew J. Nee , David Cocker
Dimethylsulfide (DMS) and dimethyldisulfide (DMDS) are precursors to products, like sulfuric acid and methanesulfonic acid (MSA), which are important to secondary aerosol formation. The formation and yields of particulate MSA and sulfuric acid from the oxidation of reduced sulfur compounds is not well understood. In this study, a 37.5 cubic meter Teflon environmental chamber was utilized to study the oxidation mechanism and aerosol forming potential of DMS and DMDS under dry conditions. Experiments were conducted in both the presence and absence of, using hydroxyl radical, nitrate radical, as well as an oxidant. With initial concentrations of 100 part-per-billion, relatively low for laboratory oxidation experiments, dominated oxidation of the reduced sulfur precursor and resulted in aerosol mass yields of greater than 40%. Hydroxyl radical oxidation of DMS and DMDS in the absence of resulted in aerosol yields of 6% and 13%, respectively, while nitrate radical oxidation in the presence of resulted in yields of 8% and less than 1%, respectively. Evidence of sulfuric acid formation was present during all particle-forming experiments, as was evidence of additional unknown sulfur-containing organic particulate. There was no evidence of MSA formation in the gas- or particle-phase throughout this study. The absence of MSA formation in the presence of has not been reported in previous studies and indicates a lack of understanding of the MSA formation mechanism. The observations made during this chamber study diverge from observations made during previous studies conducted under high precursor and concentrations, emphasizing the importance of atmospherically relevant initial conditions.
中文翻译:
表征通过还原的硫化合物氧化形成的副产物
二甲基硫醚(DMS)和二甲基二硫醚(DMDS)是产品(例如硫酸和甲磺酸(MSA))的前体,它们对二次气溶胶的形成很重要。还原性硫化合物的氧化会形成颗粒状MSA和硫酸,其收率尚不清楚。在这项研究中,使用了一个37.5立方米的特富龙环境室来研究DMS和DMDS在干燥条件下的氧化机理和气溶胶形成潜能。实验是在有或没有,也使用羟基自由基,硝酸根自由基 作为氧化剂。与最初 浓度为十亿分之十,对于实验室氧化实验而言相对较低, 还原的硫前体的氧化占主导地位,并导致气溶胶的质量产率大于40%。在不存在DMS和DMDS的情况下羟基自由基氧化 分别导致6%和13%的气溶胶收率,而在 分别导致8%的收益率和不到1%的收益率。在所有形成颗粒的实验中均存在形成硫酸的证据,以及其他未知的含硫有机颗粒的证据。在整个研究过程中,没有证据表明气相或颗粒相中有MSA形成。在存在MSA的情况下不形成MSA以前的研究尚未报道过,表明缺乏对MSA形成机理的了解。在此分庭研究期间所作的观察结果与先前在高前体和高浓度下进行的研究中所观察到的结果有所不同。 浓度,强调与大气有关的初始条件的重要性。