State Key Laboratory of Loess and Quaternary Geology, Center for Excellence in Quaternary Science and Global Change, Key Laboratory of Aerosol Chemistry & Physics, Institute of Earth Environment, Chinese Academy of Sciences, Xi'an 710061, China.
State Key Laboratory of Loess and Quaternary Geology, Center for Excellence in Quaternary Science and Global Change, Key Laboratory of Aerosol Chemistry & Physics, Institute of Earth Environment, Chinese Academy of Sciences, Xi'an 710061, China; Institute of Global Environmental Change, Xi'an Jiaotong University, Xi'an 710049, China.
Sci Total Environ. 2021 Feb 20;756:144077. doi: 10.1016/j.scitotenv.2020.144077. Epub 2020 Nov 26.
Secondary organic aerosol (SOA) is an important contributor to organic aerosol (OA), however, the model simulations of SOA concentrations and oxidation states remain significant uncertainties because of inadequate cognition of its formation and aging chemistry. In this study, SOA formation and evolution processes during summer in Xi'an were investigated, based on high-resolution online measurements of non-refractory PM (NR-PM) species and OA source apportionment using positive matrix factorization. The results showed that the total SOA, including less oxidized-oxygenated OA (LO-OOA), more oxidized-oxygenated OA (MO-OOA), and aqueous-phase-processed oxygenated OA (aq-OOA), on average constituted 69% of OA, and 43% of NR-PM, suggesting the high atmospheric oxidation capacity and the dominance of SOA during summer in Xi'an. Photochemical oxidation processes dominated the summertime SOA formation both during non-fog-rain days and fog-rain days, which were responsible for the formation of both LO-OOA and MO-OOA. Consistently, LO-OOA and MO-OOA in total contributed 59% to OA during non-fog-rain days and 56% to OA during fog-rain days, respectively. On the contrary, aq-OOA was mainly observed during fog-rain days, which increased dramatically from 2% of OA during non-fog-rain days to 19% of OA during fog-rain days with the mass concentration increasing accordingly from 0.3 μg m to 2.5 μg m. Episodic analyses further highlighted the persistently high RH period with high aerosol liquid water content (ALWC) was the driving factor of aq-OOA formation, and high O condition could further enhance its formation. Meanwhile, air masses from east and southeast were much favorable for the formation of long-time fog-rain days, which facilitated aq-OOA production during summer in Xi'an.
二次有机气溶胶(SOA)是有机气溶胶(OA)的重要贡献者,但由于对其形成和老化化学的认识不足,SOA 浓度和氧化态的模型模拟仍然存在很大的不确定性。本研究基于非挥发性颗粒物(NR-PM)物种的高分辨率在线测量和正矩阵因子化(PMF)的 OA 源解析,研究了西安夏季 SOA 的形成和演化过程。结果表明,总 SOA,包括氧化程度较低的含氧 OA(LO-OOA)、氧化程度较高的含氧 OA(MO-OOA)和水相处理的含氧 OA(aq-OOA),平均占 OA 的 69%,占 NR-PM 的 43%,表明西安夏季大气氧化能力高,SOA 占主导地位。光化学反应过程主导了夏季非雾雨日和雾雨日的 SOA 形成,这是 LO-OOA 和 MO-OOA 形成的原因。一致地,总 LO-OOA 和 MO-OOA 分别占非雾雨日 OA 的 59%和雾雨日 OA 的 56%。相反,aq-OOA 主要在雾雨日观测到,其浓度从非雾雨日的 0.3μg/m增加到雾雨日的 2.5μg/m,占 OA 的比例从非雾雨日的 2%增加到雾雨日的 19%。阶段性分析进一步强调了持续高 RH 期高气溶胶液态水含量(ALWC)是 aq-OOA 形成的驱动因素,高 O 条件可以进一步促进其形成。同时,来自东部和东南部的气团有利于长时间的雾雨天气形成,有利于西安夏季 aq-OOA 的产生。