Abstract The chemical and physical properties of secondary organic aerosol (SOA) may be influenced by the aqueous environment within which SOA-forming reactions occur. Bulk-phase reactions between glyoxal and ammonium sulfate produce light-absorbing compounds such as imidazole-2-carboxaldehyde (IC) and biimidazole (BI) and model aerosol-phase chemistry. The effect of solvent composition on IC and BI production kinetics were examined for solutions containing a series of short-chain alcohols (methanol, ethanol, 1-propanol, 2-propanol, 2-butanol, tert-butanol, and 3-methyl-2-butanol), as functions of the species and concentration added. The addition of an alcohol likely altered the solvent by inducing the formation of micro-heterogeneities of hydrated alcohol molecules. An increased alcohol concentration in solution resulted in a general increase in the production of IC and BI, with ethanol and the secondary alcohols causing the largest changes. The rate constants for IC and BI production in solutions that do not contain alcohol are found to be (4.03 ± 2.02) x 10−6 s−1 and (3.48 ± 1.75) x 10−6 s−1, respectively. In solutions that do contain an alcohol, rate constant values range from 3.23 × 10−6 s−1 to 6.61 × 10−6 s−1 for IC and 0.985 × 10−6 s−1 to 6.87 × 10−6 s−1 for BI, depending on the alcohol and the concentration. While these prevailing trends of more alcohol in solution leading to amplified production of imidazoles were observed for all seven alcohols, the diversity of responses implies the mode of action depends strongly on the species of alcohol added. Properties that describe a solution in bulk, such as dielectric constant, are not found to be reliable predictors of subsequent system behavior. Solvent composition influences SOA chemistry, and interactions between relevant functional groups within solution drive this influence, which suggests the importance of understanding individual relationships between aerosol-phase chemicals and SOA properties and production.

中文翻译：

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短链醇对乙二醛与硫酸铵本体相反应的影响

摘要 二次有机气溶胶 (SOA) 的化学和物理性质可能会受到发生 SOA 形成反应的水环境的影响。乙二醛和硫酸铵之间的本体相反应产生吸光化合物，如咪唑-2-甲醛 (IC) 和联咪唑 (BI) 和模型气溶胶相化学。对于含有一系列短链醇（甲醇、乙醇、1-丙醇、2-丙醇、2-丁醇、叔丁醇和 3-甲基-2 -丁醇），作为添加的物种和浓度的函数。添加醇可能通过诱导形成水合醇分子的微观异质性来改变溶剂。溶液中酒精浓度的增加导致 IC 和 BI 的产生普遍增加，乙醇和仲醇引起的变化最大。发现不含酒精的溶液中 IC 和 BI 产生的速率常数分别为 (4.03 ± 2.02) x 10-6 s-1 和 (3.48 ± 1.75) x 10-6 s-1。在含有酒精的溶液中，IC 的速率常数值范围为 3.23 × 10−6 s−1 到 6.61 × 10−6 s−1 和 0.985 × 10−6 s−1 到 6.87 × 10−6 s−1对于 BI，取决于酒精和浓度。虽然在所有七种醇中都观察到了溶液中更多醇导致咪唑产量增加的普遍趋势，但反应的多样性意味着作用模式在很大程度上取决于添加的醇的种类。批量描述解决方案的属性，诸如介电常数之类的指标不能作为后续系统行为的可靠预测指标。溶剂组成影响 SOA 化学，溶液中相关官能团之间的相互作用推动了这种影响，这表明了解气溶胶相化学品与 SOA 特性和生产之间的个别关系的重要性。