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化学进展 2019, Vol. 31 Issue (1): 180-190 DOI: 10.7536/PC180431 前一篇   后一篇

• 综述 •

大气半/中等挥发性有机物的组成及其对有机气溶胶贡献

唐荣志1, 王辉1, 刘莹1, 郭松1,2,**()   

  1. 1. 环境模拟与污染控制国家联合重点实验室 北京大学环境科学与工程学院 北京 100871
    2. 江苏省大气环境与装备技术协同创新中心 江苏省大气环境监测与污染控制重点实验室 南京信息工程大学 南京 210044
  • 收稿日期:2018-04-17 修回日期:2018-06-30 出版日期:2019-01-15 发布日期:2018-12-07
  • 通讯作者: 郭松
  • 基金资助:
    国家重点研发计划(2016YFC0202000); 国家重点研发计划(2017YFC0213000); 国家自然科学基金项目资助(21677002)
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Constituents of Atmospheric Semi-Volatile and Intermediate Volatility Organic Compounds and Their Contribution to Organic Aerosol

Rongzhi Tang1, Hui Wang1, Ying Liu1, Song Guo1,2,**()   

  1. 1. State Key Joint Laboratory of Environmental Simulation and Pollution Control,College of Environmental Sciences and Engineering, Peking University, Beijing 100871, China
    2. Collaborative Innovation Center of Atmospheric Environment and Equipment Technology,Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control, Nanjing University of Information Science & Technology, Nanjing 210044, China;
  • Received:2018-04-17 Revised:2018-06-30 Online:2019-01-15 Published:2018-12-07
  • Contact: Song Guo
  • About author:
    ** Corresponding author e-mail:
  • Supported by:
    The work was supported by the the National Key R&D Program of China(2016YFC0202000); The work was supported by the the National Key R&D Program of China(2017YFC0213000); The National Natural Science Foundation of China(21677002)

本文综述了大气半/中等挥发性有机物S/IVOCs的测量技术、来源、大气行为及对有机气溶胶生成的贡献。S/IVOCs测量技术的进步主要依托于质谱技术的发展,分为离线和在线测量质谱测量技术。离线测量物种鉴别能力好,但预处理复杂、时间分辨率低;在线测量技术可以获得高时间分辨率的组分及气粒分配信息,对揭示化学反应机理具有重要作用。S/IVOCs的来源包括一次和二次源。目前对一次源排放的研究主要针对机动车和生物质燃烧。研究结果表明,汽油车、柴油车和生物质燃烧排放S/IVOCs分别为POA的2.9~8.5倍、4.5~20.4倍和0.83~5.57倍。汽油车排放的S/IVOCs氧化可贡献总SOA的34%~76%,柴油车则高达90%,生物质燃烧占80%。基于外场观测数据的模型模拟表明S/IVOCs对实际大气中SOA的贡献可达40%~85%,是不可或缺的SOA前体物。未来研究中,开发新的测量技术、定量分析源排放和环境大气中S/IVOCs浓度及其对SOA贡献是研究的关键,将外场观测、实验室模拟与模型模拟相结合,能够为S/IVOCs生成SOA机制探讨提供思路。

关键词： 半/中等挥发性有机物, 测量技术, 一次排放, 二次有机气溶胶, 大气行为, 气粒分配

This review summarizes the recent advances of semi-volatile/intermediate volatility organic compounds studies, including the measurement techniques, S/IVOCs sources, atmospheric behavior and their contributions to organic aerosol formation. The rapid development of mass spectrometry facilitates the S/IVOCs measurements which include on-line and off-line mass spectrometry. The S/IVOCs off-line measurements provide more information about species at molecular level. However, the offline techniques bear the drawbacks of complex pretreatment and low time resolution, which leads to large uncertainties and the limitation to study the atmospheric chemistry processes. The on-line techniques measure the high time resolution molecular composition and gas-to-particle partitioning, and provide more useful information to elucidate the chemical mechanism of the ambient atmosphere. S/IVOCs could be directly emitted into the atmosphere, or formed by the oxidation of volatile organic compounds (VOCs). The major primary S/IVOCs sources are vehicular emission and biomass burning. Previous studies showed that ratios of S/IVOCs to POA are 2.9~8.5 for gasoline engines, 4.5~20.4 for diesel engines, and 0.83~5.57 for biomass burning. The S/IVOCs oxidation could contribute to 34%~76%, 90%, and 80% of the total SOA from the oxidation of gasoline vehicle exhaust, diesel vehicle exhaust, and biomass burning gases, respectively. Model simulation based on field observations showed that the SOA from the S/IVOCs oxidation could account for 40%~85% of the ambient SOA, suggesting that S/IVOCs are unneglectable SOA precursors. In future studies, new techniques are required to be developed to quantify more S/IVOCs species. Concentrations and speciation of S/IVOCs from different sources as well as ambient atmosphere need to be quantified. The combination of field campaign, lab study and model simulation can provide more insights of mechanism of S/IVOCs oxidation to improve our understanding of SOA formation.

Key words: semi-volatile/intermediate volatility organic compounds(S/IVOCs), measurement technique, primary emission, secondary organic aerosols, atmospheric behavior, gas-to-particle partitioning
()
图1 S/IVOCs在线测量技术,以BEACHON-RoMBAS测量为例,展示了观测期间平均碳氧化态与挥发性,并提供了非甲烷有机碳浓度信息,圆圈颜色代表相应的测量仪器信息,圆圈大小与总碳的质量成正比[32]
Fig.1 Online measurement techniques of S/IVOCs, example based on results of BEACHON-RoMBAS campaign, showing carbon oxidation state (OSc) versus volatility (c* at 298 K, μg/m3), circle area is proportional to total carbon mass, coloured by analytical technique used[32]. Copyright ? 2017, Springer Nature
表1 S/IVOCs的测量技术及优缺点
Table 1 Analytical Methods of S/IVOCs and Their Advantages and Disadvantages
Analytical
methods		 Representatives Provided information Advantages Disadvantages ref
Offline measurement GC-MS
LC-MS
GC×GC-MS		 Concentrations of organic compounds Accurate quantification
Accurate identification of molecular structure		 Complex pretreatment
Low time resolution		 33
On-line measurement TD-AMS

TD-EI-MS
TD-PTR-MS
MOVI/FIGAERO CIMS		 Total concentrations of OA, constituents and volatility
Total concentrations of S/IVOCs and volatility
Mass concentrations of organic compounds, gas to particle partitioning, volatility and molecular composition		 Low detection limit
Non pretreatment
High sensitivity
High time resolution		 Semi-quantitative
Complex calibration
Large quantity of data		 37,44
表2 S/IVOCs对SOA生成的贡献
Table 2 Contributions of S/IVOCs to SOA
Pathway Type and area Factor Contribution ref
Typical Source Emission Gasoline engines Driving cycles
NMOG/NOx
Engine technology
Emission certification standard
Exhaust aftertreatment devices		 34%~76% 52~55
Probably up to 90%
Diesel engines
As high as 85%
Biomass burning Biomass type
Season		 64
Combining field
measurement with model		 Los Angeles, USA Urban site 70%~83% 11
Forest site, USA Urban site 74%~85% 32
Pasadena, USA Urban site 88% 61
Mexico Urban site 40%~65% 66
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