北京城市大气高含氧有机分子的定量测量

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大气与环境光学学报 ›› 2020, Vol. 15 ›› Issue (6): 461-469.

• “纳米颗粒物在线测量技术”专辑 • 上一篇下一篇

北京城市大气高含氧有机分子的定量测量 #br#

陆轶群, 杨干, 刘益良, 王宇炜, 王琳∗

复旦大学环境科学与工程系, 上海 200438

收稿日期:2020-05-12 修回日期:2020-09-10 出版日期:2020-11-28 发布日期:2020-12-10
通讯作者: E-mail: lin wang@fudan.edu.cn E-mail:lin_wang@fudan.edu.cn
作者简介:陆轶群 (1990- ), 吉林舒兰人, 博士生, 主要从事大气有机物种测量方面的研究。 E-mail: yqlu16@fudan.edu.cn
基金资助:
Supported by National Key R&D Program of China (国家重点研发计划, 2017YFC0209505), National Natural Science Foundation of China (国家自然科学基金, 91644213, 21925601)

Quantitative Measurement of Highly Oxygenated Organic Molecules in Urban Beijing #br#

LU Yiqun, YANG Gan, LIU Yiliang, WANG Yuwei, WANG Lin∗ ^#br#

Department of Environmental Science and Engineering, Fudan University, Shanghai 200438, China

Received:2020-05-12 Revised:2020-09-10 Published:2020-11-28 Online:2020-12-10
Supported by:
Supported by National Key R&D Program of China (国家重点研发计划, 2017YFC0209505), National Natural Science Foundation of China (国家自然科学基金, 91644213, 21925601)

摘要/Abstract

摘要： 大气高含氧有机分子是二次有机气溶胶的重要前体物。使用气态硫酸分子作为大气高含氧有机分子的替代物评估其在硝酸根-大气常压界面化学电离飞行时间质谱离子化过程中的电离效率, 并基于高分辨率差分电迁移率粒径谱仪串联飞行时间质谱建立了质谱传输效率的矫正方法, 从而建立了大气高含氧有机分子的半定量方法。在此基础上开展了北京冬季大气高含氧有机分子的外场观测, 识别了约一百一十个大气高含氧有机分子, 表征了它们的浓度变化趋势和化学组成特征。研究发现羟基自由基在大气高含氧有机分子生成过程中具有重要作用, 而氮氧化合物也会参与其中。从挥发性分布看, 该地区冬季高含氧有机分子中归于极低挥发性有机化合物 (ELVOC) 的最多, 低挥发性有机化合物 (LVOC) 次之, 表明该地区大气高含氧有机分子在大气颗粒物上的凝结对二次有机气溶胶的形成具有重要贡献。

关键词: 高含氧有机分子, 化学电离质谱, 二次有机气溶胶, 定量方法

Abstract: Highly oxygenated organic molecules (HOMs) are important precursors for secondary organic aerosols (SOAs). Gaseous sulfuric acid was used as an analogue of HOMs to estimate the ionization efficiency of HOMs in a chemical ionization atmospheric-pressure-interface time-of-flight mass spectrometer (CI-APi-ToF) equipped with a nitrate chemical ionization source, then a mass-dependent transmission correction for HOMs was performed using a high-resolution half-mini differential mobility analyzer (HR-DMA) in tandem of the ToF-MS, and hence a semiquantitative method of atmospheric HOMs was established. Based on the method established, a field campaign was then carried out in Beijing from February to March 2018, during which about 110 HOMs species were identified together with their temporal profiles and elemental composition. The observation indicates that hydroxyl radicals play an important role in the formation of HOMs, whereas nitrogen oxides are also involved. Most of the observed HOMs can be classified as extremely low volatility organic compounds (ELVOCs), and followed by low volatility organic compounds (LVOCs), which implies that condensation of HOMs contributes to the formation of secondary organic aerosol in this particular region.

Key words: highly oxygenated organic molecules, chemical ionization mass spectrometer, secondary organic aerosol, quantitative methods

中图分类号:

陆轶群, 杨干, 刘益良, 王宇炜, 王琳∗. 北京城市大气高含氧有机分子的定量测量 #br# [J]. 大气与环境光学学报, 2020, 15(6): 461-469.

LU Yiqun, YANG Gan, LIU Yiliang, WANG Yuwei, WANG Lin∗. Quantitative Measurement of Highly Oxygenated Organic Molecules in Urban Beijing #br# [J]. Journal of Atmospheric and Environmental Optics, 2020, 15(6): 461-469.

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北京城市大气高含氧有机分子的定量测量 #br#

Quantitative Measurement of Highly Oxygenated Organic Molecules in Urban Beijing #br#

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