Acta Chim. Sinica ›› 2019, Vol. 77 ›› Issue (7): 613-624.DOI: 10.6023/A19030094 Previous Articles     Next Articles

Review

OH自由基总反应性的实地测量

杨新平a,b, 王海潮a,b, 谭照峰a,b,c, 陆克定a,b, 张远航a,b,d,e   

  1. a 北京大学环境科学与工程学院 环境模拟与污染控制国家重点实验室 北京 100871;
    b 北京大学 大气化学国际合作联合实验室 北京 100871;
    c Institute of Energy and Climate Research, IEK-8:Troposphere, Forschungszentrum Jülich GmbH, Germany 52425;
    d 中国科学院 区域大气环境研究卓越创新中心 厦门 361021;
    e 北京大学工程科学与新兴技术高精尖创新中心 北京 100871
  • 收稿日期:2019-03-21 出版日期:2019-07-15 发布日期:2019-06-03
  • 通讯作者: 陆克定, 张远航 E-mail:k.lu@pku.edu.cn;yhzhang@pku.edu.cn
  • 作者简介:杨新平,女,北京大学环境科学与工程学院2016级博士研究生,研究方向为基于OH自由基总反应性的大气HOx收支分析研究;王海潮,男,北京大学环境科学与工程学院博士后,研究方向为大气痕量在线测量技术研发和夜间大气自由基化学;谭照峰,男,德国亥姆霍兹国家研究中心联合会于利希研究中心博士后,博士毕业于北京大学环境科学与工程学院,研究方向为大气自由基化学和二次污染生成等研究
  • 基金资助:

    项目受国家自然科学基金(No.91544225)和中国大气复合污染生成的关键化学过程集成研究(No.91844301)资助.

Observations of OH Radical Reactivity in Field Studies

Yang Xinpinga,b, Wang Haichaoa,b, Tan Zhaofenga,b,c, Lu Kedinga,b, Zhang Yuanhanga,b,d,e   

  1. a State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing 100871;
    b International Joint Research Center for Atmospheric Research, Peking University, Beijing 100871;
    c Institute of Energy and Climate Research, IEK-8:Troposphere, Forschungszentrum Jülich GmbH, Jülich, Germany 52425;
    d CAS Center for Excellence in Regional Atmospheric Environment, Chinese Academy of Sciences, Xiamen 361021;
    e Beijing Innovation Center for Engineering Sciences and Advanced Technology, Peking University, Beijing 100871
  • Received:2019-03-21 Online:2019-07-15 Published:2019-06-03
  • Supported by:

    Project supported by the National Natural Science Foundation of China (No. 91544225) and Integrative study on the key chemical mechanisms of the Air Pollution Complex in China (No. 91844301).

Observations of OH Radical Reactivity in Field Studies Yang, Xinpinga,b Wang, Haichaoa,b Tan, Zhaofenga,b,c Lu, Keding*,a,b Zhang, Yuanhang*,a,b,d,e (a State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing 100871) (b International Joint Research Center for Atmospheric Research, Peking University, Beijing 100871) (c Institute of Energy and Climate Research, IEK-8:Troposphere, Forschungszentrum Jülich GmbH, Jülich, Germany 52425) (d CAS Center for Excellence in Regional Atmospheric Environment, Chinese Academy of Sciences, Xiamen 361021) (e Beijing Innovation Center for Engineering Sciences and Advanced Technology, Peking University, Beijing 100871) Abstract The hydroxyl radical (OH) is the main source of atmospheric oxidation capacity, which oxidizes the primary pollutants into the secondary pollutants. Therefore, the measurements and characterization of source and sink of OH radical are critical to understand the formation mechanism of regional secondary pollution. However, the removal routes of OH radical still cannot be quantified accurately. OH radical reactivity can describe the OH total loss rate and the atmospheric oxidation, thus playing an important role in the OH budget analysis. The OH radical reactivity is defined as the total pseudo first-order rate coefficient for all atmospheric reactions of OH in an air parcel. It is challenging to accurately measure the OH radical reactivity due to the high activity and short life of OH radical. In this paper, we summarized all kinds of measurement techniques used in the field observations of OH radical reactivity, including Total OH Loss-rate Measurement (TOHLM), Laser flash Photolysis-Laser Induced Fluorescence (LP-LIF), Chemical Ionisation Mass Spectrometry (CIMS) and Comparative Reactivity Method (CRM). The techniques were reviewed on the aspects of measurement principles, instrument modules, and so on. Overall, LP-LIF is proposed to be the best technical approach. In addition, the measured OH radical reactivity and the major scientific findings of corresponding measurement campaigns conducted in typical tropospheric conditions as urban, forest and rural environments, etc. were outlined. The OH radical reactivity varies significantly in different conditions, ranging from less than 10 per second to hundreds. Comparison of measured OH radical reactivity and the calculated or modeling results reveals a significant missing reactivity, ranging from 20% to over 80% in some environments. Depending on the emission and pollution characteristics of the field observation sites, the sources of missing reactivity are generally attributed to the undetected or unknown organic species, i.e. primary organic species, secondary organic species or a combination of both. The accurate observation and the numerical modeling of the OH radical reactivity can provide a possibility for achieving numerical closure study of ROx radicals. Finally, we discussed the current research difficulties and possible new directions for future studies of the OH radical reactivity.

Key words: OH radical reactivity, measurement techniques, field observation, compositions of OH radical reactivity, missing reactivity