Zhu Shu-Hui
Shanghai Academy of Environmental Sciences, Shanghai 200233, China.
State Environmental Protection Key Laboratory of the Formation and Prevention of Urban Air Pollution Complex, Shanghai 200233, China.
Huan Jing Ke Xue. 2023 Jul 8;44(7):3760-3770. doi: 10.13227/j.hjkx.202208259.
Organic aerosols (OA) are closely related to the formation of both PM and O in the atmosphere. In this study, a thermal desorption aerosol GC/MS (TAG) online system was adopted to measure hourly concentrations of 94 total organic molecular markers in PM at an urban site in Shanghai from November 6 to December 31, 2021. Combined with air mass cluster analysis and other online measurement data, the chemical characteristics of OA under the influence of different air masses, oxidant levels, and relative humidity (RH) levels were investigated. The results showed that OA was characterized by higher mass percentages of primary organic molecular markers (e.g., saturated fatty acids, unsaturated fatty acids, and alkanes) under the influence of local air masses. Further, high loadings of biomass burning tracers were observed in OA under the influence of long-range transported air masses. In contrast, OA impacted by marine air masses was laden with significantly higher fractions of secondary organic molecular markers, such as dicarboxylic acids and hydroxyl dicarboxylic acids, which were formed from a wide range of volatile organic precursors through photochemical and aqueous-phase processing. With the application of the positive matrix factorization (PMF) model, seven total primary source factors and five secondary source factors were resolved for PM and OA during the observation. Among them, secondary nitrate was the highest contributor to PM mass with a mass percentage of 25.2%, whereas vehicle emissions were the top contributor (24.0%) to OA mass. Primary source factors, including coal combustion, vehicle emission, and cooking emission as well as their corresponding secondary source factors (e.g., secondary nitrate, secondary organic aerosols 2, etc.) showed elevated contributions in PM and OA with the increase in PM masses, indicating that more stringent controls of local emission sources (e.g., coal combustion, vehicle emission, and cooking emission) are needed to further lower PM pollution and improve air quality in Shanghai.
有机气溶胶(OA)与大气中颗粒物(PM)和臭氧(O)的形成密切相关。本研究采用热脱附气溶胶气相色谱/质谱联用(TAG)在线系统,于2021年11月6日至12月31日在上海某城市站点每小时测量一次PM中94种总有机分子标志物的浓度。结合气团聚类分析和其他在线测量数据,研究了不同气团、氧化剂水平和相对湿度(RH)水平影响下OA的化学特征。结果表明,在本地气团影响下,OA的特征是初级有机分子标志物(如饱和脂肪酸、不饱和脂肪酸和烷烃)的质量百分比更高。此外,在远距离传输气团影响下的OA中观察到生物质燃烧示踪剂的高负荷。相比之下,受海洋气团影响的OA中含有显著更高比例 的二次有机分子标志物,如二元羧酸和羟基二元羧酸,它们是由多种挥发性有机前体通过光化学和水相过程形成的。通过应用正定矩阵因子分解(PMF)模型,在观测期间解析出了PM和OA的七个主要源因子和五个二次源因子。其中,二次硝酸盐对PM质量的贡献最大,质量百分比为25.2%,而车辆排放是OA质量的最大贡献者(24.0%)。包括煤炭燃烧、车辆排放和烹饪排放在内的主要源因子及其相应的二次源因子(如二次硝酸盐、二次有机气溶胶2等)随着PM质量的增加在PM和OA中的贡献增加,这表明需要更严格地控制本地排放源(如煤炭燃烧、车辆排放和烹饪排放),以进一步降低上海的PM污染并改善空气质量。