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在北京市雾霾期间,萘和甲基萘的气相氧化对二次有机气溶胶可能有重要贡献。

Potentially Important Contribution of Gas-Phase Oxidation of Naphthalene and Methylnaphthalene to Secondary Organic Aerosol during Haze Events in Beijing.

机构信息

SKL-ESPC and BIC-ESAT, College of Environmental Sciences and Engineering , Peking University , Beijing 100871 , China.

Institute for Environmental and Climate Research , Jinan University , Guangzhou 511443 , China.

出版信息

Environ Sci Technol. 2019 Feb 5;53(3):1235-1244. doi: 10.1021/acs.est.8b04523. Epub 2019 Jan 24.

DOI:10.1021/acs.est.8b04523
PMID:30625271
Abstract

Naphthalene (Nap) and methylnaphthalene (MN) are the most abundant polycyclic aromatic hydrocarbons (PAHs) in atmosphere and have been proposed to be important precursors of anthropogenic secondary organic aerosol (SOA) derived from laboratory chamber experiments. In this study, atmospheric Nap/MN and their gas-phase photooxidation products were quantified by a Proton Transfer Reaction-Quadrupole interface Time-of-Flight Mass Spectrometer (PTR-QiTOF) during the 2016 winter in Beijing. Phthalic anhydride, a late generation product from Nap under high-NO conditions, appeared to be more prominent than 2-formylcinnamaldehyde (early generation product), possibly due to more sufficient oxidation during the haze. 1,2-Phthalic acid (1,2-PhA), the hydrated form of phthalic anhydride, was capable of partitioning into aerosol phase and served as a tracer to explore the contribution of Nap to ambient SOA. The measured fraction in particle phase ( F) of 1,2-PhA averaged at 73 ± 13% with OA mass loadings of 52.5-87.8 μg/m, lower than the value predicted by the absorptive partitioning model (100%). Using tracer product-based and precursor consumption-based methods, 2-ring PAHs (Nap and MN) were estimated to produce 14.9% (an upper limit) of the SOA formed in the afternoon during the wintertime haze, suggesting a comparable contribution of Nap and MN with monocyclic-aromatics on urban SOA formation.

摘要

萘(Nap)和甲基萘(MN)是大气中最丰富的多环芳烃(PAHs),并被提议作为人为二次有机气溶胶(SOA)的重要前体,这些 SOA 源自实验室腔室实验。在这项研究中,2016 年冬季在北京,通过质子转移反应-四极杆接口飞行时间质谱仪(PTR-QiTOF)定量测定了大气中 Nap/MN 及其气相光氧化产物。邻苯二甲酸酐是 Nap 在高 NO 条件下的晚期产物,似乎比 2-糠醛(早期产物)更为突出,这可能是由于在雾霾期间有更充分的氧化作用。1,2-邻苯二甲酸(1,2-PhA)是邻苯二甲酸酐的水合形式,能够分配到气溶胶相中,并作为示踪剂来探索 Nap 对环境 SOA 的贡献。在 52.5-87.8μg/m 的 OA 质量负荷下,1,2-PhA 在颗粒相中( F)的测量分数平均为 73±13%,低于吸收分配模型(100%)预测的值。使用示踪剂产物法和前体消耗法,估计 2-环 PAHs(Nap 和 MN)在冬季雾霾期间下午形成的 SOA 中占 14.9%(上限),表明 Nap 和 MN 与单环芳烃对城市 SOA 形成的贡献相当。

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