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光氧化芳香烃生成二次有机气溶胶老化的烟雾箱/氧化流动反应器联合研究。

Combined Smog Chamber/Oxidation Flow Reactor Study on Aging of Secondary Organic Aerosol from Photooxidation of Aromatic Hydrocarbons.

机构信息

State Key Joint Laboratory of Environment Simulation and Pollution Control, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China.

Center for Excellence in Regional Atmospheric Environment, Institute of Urban Environment, Chinese Academy of Sciences, Xiamen 361021, China.

出版信息

Environ Sci Technol. 2023 Sep 19;57(37):13937-13947. doi: 10.1021/acs.est.3c04089. Epub 2023 Sep 10.

Abstract

Secondary organic aerosol (SOA) is a significant component of atmospheric fine particulate matter (PM), and their physicochemical properties can be significantly changed in the aging process. In this study, we used a combination consisting of a smog chamber (SC) and oxidation flow reactor (OFR) to investigate the continuous aging process of gas-phase organic intermediates and SOA formed from the photooxidation of toluene, a typical aromatic hydrocarbon. Our results showed that as the OH exposure increased from 2.6 × 10 to 6.3 × 10 molecules cm s (equivalent aging time of 2.01-4.85 days), the SOA mass concentration (2.9 ± 0.05-28.7 ± 0.6 μg cm) and corrected SOA yield (0.073-0.26) were significantly enhanced. As the aging process proceeds, organic acids and multiple oxygen-containing oxidation products are continuously produced from the photochemical aging process of gas-phase organic intermediates (mainly semi-volatile and intermediate volatility species, S/IVOCs). The multigeneration oxidation products then partition to the aerosol phase, while functionalization of SOA rather than fragmentation dominated in the photochemical aging process, resulting in much higher SOA yield after aging compared to that in the SC. Our study indicates that SOA yields as a function of OH exposure should be considered in air quality models to improve SOA simulation, and thus accurately assess the impact on SOA properties and regional air quality.

摘要

二次有机气溶胶(SOA)是大气细颗粒物(PM)的重要组成部分,其物理化学性质在老化过程中会发生显著变化。在这项研究中,我们使用了一个包含烟雾箱(SC)和氧化流动反应器(OFR)的组合,来研究甲苯光氧化过程中气相有机中间产物和 SOA 的连续老化过程,甲苯是一种典型的芳烃。我们的结果表明,随着 OH 暴露量从 2.6×10增加到 6.3×10分子 cm s(等效老化时间从 2.01 到 4.85 天),SOA 质量浓度(2.9±0.05-28.7±0.6μg cm)和修正后的 SOA 产率(0.073-0.26)显著增加。随着老化过程的进行,有机酸和多种含氧氧化产物不断从气相有机中间产物的光化学老化过程中产生(主要是半挥发性和中等挥发性物质,S/IVOCs)。多代氧化产物随后分配到气溶胶相,而在光化学老化过程中,SOA 的功能化而不是碎片化占主导地位,导致老化后的 SOA 产率比 SC 中的产率高得多。我们的研究表明,空气质量模型中应考虑 SOA 产率与 OH 暴露量的函数关系,以改善 SOA 模拟,从而准确评估对 SOA 性质和区域空气质量的影响。

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