Synergistic Effects of SO2 and NH3 Coexistence on SOA Formation from Gasoline Evaporative Emissions.
Synergistic Effects of SO2 and NH3 Coexistence on SOA Formation from Gasoline Evaporative Emissions.
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DOI：
10.1021/acs.est.3c01921
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发表时间：
2023-04
影响因子：
11.4
通讯作者：
Tianzeng Chen;P. Zhang;Biwu Chu;Qingxin Ma;Y. Ge;Hong S. He
中科院分区：
文献类型：
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作者：
Tianzeng Chen;P. Zhang;Biwu Chu;Qingxin Ma;Y. Ge;Hong S. He
车辆蒸发排放对挥发性有机化合物（VOCs）的人为来源的贡献越来越大，从而促进了二次有机气溶胶（SOA）的形成。然而，在NOx、SO2和NH3共存的复杂污染条件下，车辆挥发性VOCs形成SOA的研究很少。本研究利用30 m3雾霾室，借助一系列质谱仪，考察了SO2和NH3对汽油挥发性VOCs与NOx形成SOA的协同效应。与单独存在SO2或NH3的体系相比，SO2和NH3共存对SOA形成的促进作用更大，且大于单独存在两种促进作用的累积效应。同时，对比了有NH3和无NH3时SO2对SOA氧化态（OSc）的影响，当有NH3存在时SO2可以进一步提高OSc。后者归因于SO2和NH3共存对SOA形成的协同作用，其中SO2与NH3存在下生成的n -杂环反应可形成N-S-O加合物。我们的研究有助于理解高度复杂污染条件下车辆蒸发挥发性有机化合物形成SOA及其对大气的影响。
Vehicular evaporative emissions make an increasing contribution to anthropogenic sources of volatile organic compounds (VOCs), thus contributing to secondary organic aerosol (SOA) formation. However, few studies have been conducted on SOA formation from vehicle evaporative VOCs under complex pollution conditions with the coexistence of NOx, SO2, and NH3. In this study, the synergistic effects of SO2 and NH3 on SOA formation from gasoline evaporative VOCs with NOx were examined using a 30 m3 smog chamber with the aid of a series of mass spectrometers. Compared with the systems involving SO2 or NH3 alone, SO2 and NH3 coexistence had a greater promotion effect on SOA formation, which was larger than the cumulative effect of the two promotions alone. Meanwhile, contrasting effects of SO2 on the oxidation state (OSc) of SOA in the presence or absence of NH3 were observed, and SO2 could further increase the OSc with the coexistence of NH3. The latter was attributed to the synergistic effects of SO2 and NH3 coexistence on SOA formation, wherein N-S-O adducts can be formed from the reaction of SO2 with N-heterocycles generated in the presence of NH3. Our study contributes to the understanding of SOA formation from vehicle evaporative VOCs under highly complex pollution conditions and its atmospheric implications.