State Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou, Guangdong 510640. China.
CAS Center for Excellence in Deep Earth Science, Guangzhou, Guangdong 510640, China.
Environ Sci Technol. 2022 Jun 7;56(11):6880-6893. doi: 10.1021/acs.est.1c03155. Epub 2021 Dec 13.
Oxygenated volatile organic compounds (OVOCs) and secondary organic aerosol (SOA) formation potential of ambient air in Guangzhou, China was investigated using a field-deployed oxidation flow reactor (OFR). The OFR was used to mimic hours to weeks of atmospheric exposure to hydroxyl (OH) radicals within the 2-3 min residence time. A comprehensive investigation on the variation of VOCs and OVOCs as a function of OH exposure is shown. Substantial formation of organic acids and nitrogen-containing OVOC species were observed. Maximum SOA formation in the OFR was observed following 1-4 equiv days' OH exposure. SOA produced from known/measured VOC/IVOC precursors such as single-ring aromatics and long-chain alkanes can account for 52-75% of measured SOA under low NO and 26-60% under high NO conditions based on laboratory SOA yield parametrizations. To our knowledge, this is the first time that the contribution (8-20%) of long-chain (C-C) alkane oxidation to OFR SOA formation was quantified from direct measurement. By additionally estimating contribution from unmeasured semivolatile and intermediate volatility compounds (S/IVOCs) that are committed with C-C alkanes, 64-100% of the SOA formation observed in the OFR can be explained, signifying the important contribution of S/IVOCs such as large cyclic alkanes to ambient SOA.
使用现场部署的氧化流动反应器 (OFR) 研究了中国广州环境空气中含氧挥发性有机化合物 (OVOC) 和二次有机气溶胶 (SOA) 的形成潜力。OFR 用于模拟大气中羟基 (OH) 自由基在 2-3 分钟停留时间内数小时到数周的暴露。展示了对 VOC 和 OVOC 随 OH 暴露变化的综合研究。观察到有机酸和含氮 OVOC 物种的大量形成。在 1-4 当量/天 OH 暴露后,OFR 中观察到最大的 SOA 形成。基于实验室 SOA 产率参数化,已知/测量的 VOC/IVOC 前体(如单环芳烃和长链烷烃)产生的 SOA 可占低 NO 条件下测量到的 SOA 的 52-75%,高 NO 条件下占 26-60%。据我们所知,这是首次从直接测量中定量出长链 (C-C) 烷烃氧化对 OFR SOA 形成的贡献 (8-20%)。通过另外估算与 C-C 烷烃相关的未测量半挥发性和中等挥发性化合物 (S/IVOC) 的贡献,可解释 OFR 中观察到的 SOA 形成的 64-100%,表明 S/IVOC (如大环状烷烃)对环境 SOA 的重要贡献。