Damianos Pavlidis, Petro Uruci, Kalliopi Florou, Andrea Simonati, Christina Ν Vasilakopoulou, Georgia Argyropoulou, Spyros N Pandis
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引用次数: 0
摘要
研究了人为大挥发性有机化合物(VOC)和中间挥发性有机化合物(IVOC)在高氮氧化物条件下与羟基自由基反应产生的二次有机气溶胶(SOA)。所研究的有机化合物包括体积不断增大的环状烷烃(戊基环己烷、己基环己烷、壬基环己烷和癸基环己烷)和芳香族化合物(1,3,5-三甲苯、1,3,5-三甲苯和 1,3,5-三叔丁基苯)。所有研究化合物都形成了大量的 SOA。对于所研究的环己烷(C11-C16),SOA 产量似乎与替代链的长度呈非线性关系。大环己烷的产率高于芳香族化合物,但芳香族前体产生的氧化 SOA 更多。这是由于环己烷产生了挥发性较低的 O:C 第一代产物。环己烷的大多数氧化产物(C* < 104 μg m-3)都是 SVOC(50%),而芳烃则是 IVOC(60%)。研究发现,母体碳氢化合物的结构、分子大小和替代链长度对 SOA 的形成、氧化态和挥发性起着关键作用。通过结合 SOA 产量、热扩散(TD)和等温稀释测量,还对 SOA 的挥发性分布、有效汽化焓和有效容纳系数进行了量化。此外,还提出了挥发性基础集(VBS)的参数设置,以供将来在化学传输模型中使用。
Secondary Organic Aerosol Formation during the Oxidation of Large Aromatic and Other Cyclic Anthropogenic Volatile Organic Compounds.
The secondary organic aerosol (SOA) production from the reactions of anthropogenic large volatile (VOCs) and intermediate volatility organic compounds (IVOCs) with hydroxyl radicals under high NO x conditions was investigated. The organic compounds studied include cyclic alkanes of increasing size (amylcyclohexane, hexylcyclohexane, nonylcyclohexane, and decylcyclohexane) and aromatic compounds (1,3,5-trimethylbenzene, 1,3,5-triethylbenzene and 1,3,5-tritert-butylbenzene). A considerable amount of SOA was formed from all examined compounds. For the studied cyclohexanes (C11-C16) there appears that the SOA yield depends nonlinearly on the length of their substitute chain. The large cyclohexanes had higher yields than the aromatic compounds, but the aromatic precursors produced a more oxidized SOA. This was due to the production of lower volatility and O:C first generation products by the cyclohexanes. Most oxidation products (with C* < 104 μg m-3) in the case of cyclohexanes are SVOCs (∼50%), while of aromatics are IVOCs (∼60%). Structure, molecular size, and length of the substitute chain of the parent hydrocarbon were found to play key roles in SOA formation, oxidation state, and volatility. The SOA volatility distribution, effective vaporization enthalpy, and effective accommodation coefficient were also quantified by combining SOA yields, thermodenuder (TD) and isothermal dilution measurements. Parameterizations for the Volatility Basis Set (VBS) are proposed for future use in chemical transport models.