Department of Chemistry and Biochemistry, University of San Diego , 5998 Alcalá Park, San Diego California 92110, United States.
Environ Sci Technol. 2014 Dec 16;48(24):14417-25. doi: 10.1021/es5044479. Epub 2014 Dec 3.
Reactions of carbonyl compounds in cloudwater produce organic aerosol mass through in-cloud oxidation and during postcloud evaporation. In this work, postcloud evaporation was simulated in laboratory experiments on evaporating droplets that contain mixtures of common atmospheric aldehydes with ammonium sulfate (AS), methylamine, or glycine. Aerosol diameters were measured during monodisperse droplet drying experiments and during polydisperse droplet equilibration experiments at 75% relative humidity, and condensed-phase mass was measured in bulk thermogravimetric experiments. The evaporation of water from a droplet was found to trigger aldehyde reactions that increased residual particle volumes by a similar extent in room-temperature experiments, regardless of whether AS, methylamine, or glycine was present. The production of organic aerosol volume was highest from droplets containing glyoxal, followed by similar production from methylglyoxal or hydroxyacetone. Significant organic aerosol production was observed for glycolaldehyde, acetaldehyde, and formaldehyde only at elevated temperatures in thermogravimetric experiments. In many experiments, the amount of aerosol produced was greater than the sum of all solutes plus nonvolatile solvent impurities, indicating the additional presence of trapped water, likely caused by increasing aerosol-phase viscosity due to oligomer formation.
羰基化合物在云中的反应通过云内氧化和云后蒸发产生有机气溶胶质量。在这项工作中,通过在含有常见大气醛与硫酸铵(AS)、甲胺或甘氨酸混合物的蒸发液滴的实验室实验中模拟了云后蒸发。在单分散液滴干燥实验和在 75%相对湿度下的多分散液滴平衡实验中测量了气溶胶直径,并在批量热重实验中测量了凝聚相质量。发现从液滴中蒸发水会引发醛反应,这些反应在室温实验中以相似的程度增加了残余颗粒体积,无论 AS、甲胺还是甘氨酸是否存在。含有乙二醛的液滴产生的有机气溶胶体积最高,其次是甲基乙二醛或羟基丙酮产生的类似体积。仅在热重实验中的高温下才观察到乙二醇醛、乙醛和甲醛产生明显的有机气溶胶。在许多实验中,产生的气溶胶量大于所有溶质加不可挥发溶剂杂质的总和,表明存在额外的被困水,这可能是由于形成低聚物导致气溶胶相粘度增加所致。