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化学进展 2022, Vol. 34 Issue (9): 2094-2107 DOI: 10.7536/PC211215 前一篇   后一篇

• 综述 •

大气中的单环芳香族硝基化合物

薛宗涵1,2,3, 马楠1,3,*(), 王炜罡2,*()   

  1. 1 暨南大学环境与气候研究院 广州 511443
    2 中国科学院化学研究所 分子动态与稳态结构实验室 北京 100190
    3 粤港澳环境质量协同创新联合实验室 广州 511443
  • 收稿日期:2022-12-10 修回日期:2022-02-16 出版日期:2022-09-20 发布日期:2022-04-01
  • 作者简介:

    马楠 暨南大学环境与气候研究院研究员,博士生导师,主要研究方向有黑碳气溶胶、气溶胶-云相互作用、气溶胶观测技术研发等,已在Science、Proc. Natl. Acad. Sci.等国际高水平期刊发表SCI论文70余篇。

    王炜罡 中国科学院化学研究所研究员,主要研究方向有VOCs大气化学、二次气溶胶、气溶胶物理化学性质、大气化学动力学等,已在Nature Communications等国际高水平期刊发表SCI论文80余篇。

  • 基金资助:
    广东省“珠江人才计划”引进创新创业团队项目(2016ZT06N263); 广东省科技创新战略专项资金项目(2019B121205004)
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Nitrated Mono-Aromatic Hydrocarbons in the Atmosphere

Zonghan Xue1,2,3, Nan Ma1,3(), Weigang Wang2()   

  1. 1 Institute for Environmental and Climate Research, Jinan University,Guangzhou 511443, China
    2 State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences,Beijing 100190, China
    3 Guangdong-Hongkong-Macau Joint Laboratory of Collaborative Innovation for Environmental Quality,Guangzhou 511443, China
  • Received:2022-12-10 Revised:2022-02-16 Online:2022-09-20 Published:2022-04-01
  • Contact: *e-mail: wangwg@iccas.ac.cn (Weigang Wang);nan.ma@jnu.edu.cn (Nan Ma)
  • Supported by:
    Guangdong Innovative and Entrepreneurial Research Team Program(2016ZT06N263); Special Fund Project for Science and Technology Innovation Strategy of Guangdong Province(2019B121205004)

单环芳香族硝基化合物(Nitrated mono-aromatic hydrocarbons,NMAHs)是大气中备受研究关注的一类物质,其同系物种类繁多且理化性质具有显著差异。随着研究技术的进步,外场观测能识别更丰富的NMAHs物种,实验室研究也逐渐能揭示不同NMAHs物种的生成机制。基于此,本文调研了过去近15年国内外已发表有关大气中NMAHs的文献。我们首先归纳和梳理了大气NMAHs在欧洲地区和中国地区以及其他地区的时空分布、主要来源、“气-粒”分配等特征。其次,我们结合实验室实验和外场观测结果总结了NMAHs的生成及损耗机制,并探讨了在光吸收特性、环境健康效应以及相关测量技术等方面的研究进展。最后,本文总结并提出大气NMAHs研究中仍需要解决的科学问题和未来可能的研究方向。

关键词： 单环芳香族硝基化合物, 时空分布, “气-粒”分配, 生成与损耗机制, 光吸收特性, 环境健康效应

Nitrated mono-aromatic hydrocarbons(NMAHs)are a class of pollutants with a wide variety of homologous species and complex physical and chemical properties,which are getting increasingly concerned in the researches of atmospheric chemistry.With the advance of measurement technology,more and more types of NMAHs species can be identified in field observations,and the generation mechanisms of different NMAHs are revealed in laboratory research.Base on this, we collected the published literatures of domestic and foreign research in the past 15 years on NMAHs in this paper. Firstly, We summarized its characteristics of temporal and spacial distribution, main sources, gas-particle partitioning in Europe and China as well as other places. Secondly, combing with laboratory experiments and field observations, we summarized generation and loss mechanism of NMAHs,and discussed the research progress in optical absorption, environment and health effects, as well as measurement techniques. Finally, the important scientific problems that need to be solved and future potential research directions are summarized.

Contents

1 Introduction

2 Emission and distribution characteristics of NMAHs in the atmosphere

2.1 Temporal and spatial distribution

2.2 Main sources

2.3 Gas-particle partitioning

3 Mechanisms of generation and loss of NMAHs

3.1 Mechanisms of generation and loss in gas phase

3.2 Mechanisms of generation in particle phase

4 Optical absorption of NMAHs

5 Environment and health effects of NMAHs

6 Measurement technology of NMAHs

6.1 Outline measurement technology

6.2 Online measurement technology

7 Conlusions and outlook

Key words: nitrated mono-aromatic hydrocarbons, temporal and special distribution, gas-particle partitioning, generation and loss mechanism, optical absorption, environment and health effects
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表1 文献报道的国内外外场观测中NMAHs浓度及其季节变化
Table 1 The concentration of NMAHs and their seasonal variation in domestic and foreign field observations reported in the literatures
Country Contents(ng/m3) Observation Types
(Locaion)		 Observation Time
Annual Winter Autumn Spring Summer
France[32] NMAHs Urban(Strasbourg) 25.2 21.6 26.1~28.4 18.2~31.7
Suburb(Schiltigheim) 23.5 24.8~29.6 16.1
Rural(Erstein) 21.1 22.7 19.5
Slovenia[27] NMAHs Urban(Ljubljana) 150.59 1.16
China[5] NMAHs Urban(Hong Kong) 3.34~19.73 5.31~7.70 1.01~3.57 0.28~3.28
China[12] NMAHs Urban(Jinan) 105.4 34 13.5
China[38] NMAHs Urban(Jinan) 48.4 9.8
Rural(Wangdu,Yucheng) 5.7~5.9
Mt. Tai 2.5
China[40] NMAHs Rural (Mt. Tai) 14.1 8.5
China[36] NMAHs Urban(Nanjing) 18.77 44.79 17.28 16.82 8.59
China[35] NMAHs Urban(Shanghai) 22.4 9.84 9.31 4.16
Germany[3] NMAHs(ng/L) Urban(Mainz) 278.74~4252.6
Rural(Winterberg,Altenberg) 696.12~
1303.73
Austria[3] NMAHs(ng/L) Urban(Götzens) 1264.35
Rural(Kolsassberg) 809.95
Czech Republic[3] NMAHs(ng/L) Urban(Ostrava) 635.43
Rural(Pustá Polom) 1128.58~
1210.59
Norge[3] NMAHs(ng/L) Remote(Arctic,Tempelfjorden,
Svalbard)		 390.5
Czech Republic[4] NMAHs Urban(Ostrava,Kladno) 93~102 8.8
Belgium[9] NMAHs Rural(Flanders) 6.42 32.19 12.71 3.78 2.16
China[8] NMAHs Urban(Beijing) 6.63
Canada[37] 4NP Urban(Hamilton) 0.729
Rural(Simcoe) 0.408
Hungary[18] 4NC Urban(Budapest) 8.5 0.5
Rural(K-puszta) 0.3
Brazil[18] 4NC Rainforest(Rondônia,day/night) 97/520
表2 NMAHs物种与左旋葡聚糖的相关性
Table 2 Correlation between NMAHs and levoglucan
Compounds R value Observation
period		 Location
(4NP+3M4NP+2M4NP+2,6DNP) 0.77 Winter Hong Kong,China[5]
0.8 Spring
0.45 Summer
0.85 Autumn
(4NC+4M5NC+3M6NC+3M5NC) 0.83 Winter Hong Kong,China[5]
0.71 Spring
0.57 Summer
0.48 Autumn
(4M5NC+3M6NC+3M5NC) 0.749 Winter Seiffen and
Saxony,Germany[23]
4NC 0.71 Campain Flanders,Belgium[9]
MNCs 0.66 Campain
DMNCs 0.65 Campain
4NP 0.64 Campain Shanghai,China[24]
4NG -0.12 Campain
4NC 0.72 Campain
NMAHs 0.82 Campain Hong Kong,China[5]
图1 春夏季颗粒相NMAHs物种占比[12]
Fig. 1 The fractions of NMAHs species in particle phase in spring and summer[12]
图2 NMAHs物种在气相和颗粒相中生成及迁移的途径(以部分物种为例)[8,16,25,28,62⇓~64]
Fig. 2 The pathways by which NMAHs species are generated and migrated in the gas phase and particle phase(take some species as an example)[8,16,25,28,62⇓~64]
表3 部分NMAHs物种的最大吸收波长[1]
Table 3 The maximum absorption wavelength of some NMAHs species[1]
Compound m/Q detected,
deprotonated(Th)		 mean concention (ng·m-3) λmax(nm)
4NP 138.019 0.02 317
4M2NP 152.035 5 319
4NC 154.014 2.5 337
2,4DNP 183.004 3 292
表1 物质名称
中文名称 英文名称 英文缩略语
单环芳香族硝基化合物 Nitrated Mono-aromatic Hydrocarbons NMAHs
硝基苯酚类 Nitrophenols NPs
硝基苯酚类甲基衍生物 Methy-Nitrophenols MNPs
硝基儿茶酚类 Nitrocatechols NCs
硝基儿茶酚类甲基衍生物 Methy-Nitrocatechols MNCs
二硝基苯酚类 Dinitrophenols DNPs
二硝基苯酚类甲基衍生物 Methy-Dinitrophenols MDNPs
硝基水杨酸类 Nitrosalicylic Acids NSAs
硝基愈创木酚类 Nitroguaiacols NGs
4-硝基儿茶酚 4-Nitrocatechol 4NC
4-硝基苯酚 4-Nitrophenol 4NP
3-甲基-4-硝基苯酚 3-Methy-4-Nitrophenol 3M4NP
2-甲基-4-硝基苯酚 2-Methy-4-Nitrophenol 2M4NP
3-硝基水杨酸 3-Nitrosalicylic Acid 3NSA
5-硝基水杨酸 5-Nitrosalicylic Acid 5NSA
4-硝基愈创木酚 4-Nitroguaiacol 4NG
2-硝基苯酚 2-Nitrophenol 2NP
3-甲基-6-硝基儿茶酚 3-Methy-6-Nitrocatechol 3M6NC
3-甲基-5-硝基儿茶酚 3-Methy-5-Nitrocatechol 3M5NC
4-甲基-5-硝基儿茶酚 4-Methy-5-Nitrocatechol 4M5NC
2,4-二硝基苯酚 2,4-Dinitrophenol 2,4DNP
4-甲基-2,6-二硝基苯酚 4-Methy-2,6-Dinitrophenol 4M2,6DNP
2,6-二甲基-4-硝基苯酚 2,6-Dimethy-4-Nitrophenol 2,6DM4NP
4-甲基-2-硝基苯酚 4-Methy-2-Nitrophenol 4M2NP
5-甲基-2-硝基苯酚 5-Methy-2-Nitrophenol 5M2NP
4,6-二硝基愈创木酚 4,6-Dinitroguaiacol 4,6DNG
5-硝基愈创木酚 5-Nitroguaiacol 5NG
3-甲基儿茶酚 3-Methycatechol 3MC
4-甲基儿茶酚 4-Methycatechol 4MC
3-甲基硝基儿茶酚类 3-Methy-Nitrocatechols 3MNCs
愈创木酚 Guaiacol GUA
6-硝基愈创木酚 6-Nitroguaiacol 6NG
表2 仪器名称
中文名称 英文名称 英文缩略语
努森池扩散质谱仪 Knudsen Effusion Mass Spectrometry KEMS
化学电离质谱仪 Chemical Ionization Mass Spectrometer CIMS
液相色谱串联质谱 Liquid Chromatography/Mass Spectrometry LC/MS
液相色谱/电喷雾电离线性离子阱质谱 Liquid Chromatography/Electrospray Ionization
Linear Ion Trap Mass Spectrometry		 LC/ESI-LITMS
高效液相色谱/高分辨率四极杆飞行时间质谱 Ultra Performance Liquid Chromatography/
Electrospray Ionization Quadrupole
Time-of-Flight Mass Spectrometry		 UPLC/ESI-Q-TOF-MS
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摘要

大气中的单环芳香族硝基化合物