School of Interdisciplinary Research, Indian Institute of Technology Delhi, Delhi, 110016, India; Department of Mechanical Engineering, Indian Institute of Technology Delhi, Delhi, 110016, India.
Atmospheric Chemistry Department, Max Planck Institute for Chemistry, Mainz, 55128, Germany; Physical Research Laboratory, Navrangpura, Ahmedabad, 380009, India.
Environ Res. 2024 Jun 15;251(Pt 1):118542. doi: 10.1016/j.envres.2024.118542. Epub 2024 Feb 23.
Secondary aerosols constitute a significant fraction of atmospheric aerosols, yet our understanding of their formation mechanism and fate is very limited. In this work, the secondary organic aerosol (SOA) formation and aging of ambient air of Delhi are studied using a potential aerosol mass (PAM) reactor, an oxidation flow reactor (OFR), coupled with aerosol chemical speciation monitor (ACSM), proton transfer reaction time of flight mass spectrometer (PTR-ToF-MS), and scanning mobility particle sizer with counter (SMPS + C). The setup mimics atmospheric aging of up to several days with the generation of OH radicals. Variations in primary volatile organic compounds (VOCs) and oxygenated volatile organic compounds (OVOCs) as a function of photochemical age were investigated. Primary VOCs such as benzene, toluene, xylene, trimethyl benzene, etc. decrease and OVOCs like formic acid, formaldehyde, acetone, ethanol, etc. increase substantially upon oxidation in OFR. The highest organic aerosol (OA) enhancement was observed for the 4.2 equivalent photochemical days of aging i.e., 1.84 times the ambient concentration, and net OA loss was observed at very high OH exposure, typically after 8.4 days of photochemical aging due to heterogeneous oxidation followed by fragmentation/evaporation. In ambient air, OA enhancement is highest during nighttime due to the high concentrations of precursor VOCs in the atmosphere. SMPS + C results demonstrated substantial new particle formation upon aging and decrement in preexisting aerosol mass. This is the first experimental study conducting an in-situ evaluation of potential SOA mass generated from the ambient aerosols in India.
二次气溶胶构成了大气气溶胶的重要组成部分,但我们对其形成机制和归宿的了解非常有限。在这项工作中,使用潜在气溶胶质量(PAM)反应器、氧化流动反应器(OFR)以及气溶胶化学特征监测器(ACSM)、质子转移反应飞行时间质谱仪(PTR-ToF-MS)和带有计数器的扫描迁移率颗粒物粒径谱仪(SMPS+C)研究了德里环境空气中的二次有机气溶胶(SOA)形成和老化。该装置模拟了长达数天的大气老化过程,并产生了 OH 自由基。研究了作为光化学年龄函数的初始挥发性有机化合物(VOC)和含氧挥发性有机化合物(OVOC)的变化。在 OFR 中氧化时,苯、甲苯、二甲苯、三甲苯等主要 VOC 会减少,甲酸、甲醛、丙酮、乙醇等 OVOC 会大量增加。在 4.2 个等效光化学老化天数(即 1.84 倍环境浓度)下观察到最高的有机气溶胶(OA)增强,并且在非常高的 OH 暴露下观察到净 OA 损失,通常在 8.4 天的光化学老化后由于异相氧化 followed by fragmentation/evaporation。在环境空气中,由于大气中前体 VOC 浓度较高,OA 增强在夜间最高。SMPS+C 结果表明,老化后会发生大量新粒子形成,并且预先存在的气溶胶质量会减少。这是首次在印度对环境气溶胶中潜在 SOA 质量进行现场评估的实验研究。