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化学进展 2021, Vol. 33 Issue (1): 151-161 DOI: 10.7536/PC200958 前一篇   

• 综述 •

大气中活性气态汞的分析方法和赋存转化

方莹莹1,2, 王颖1,2, 史建波1,2,4, 阴永光1,2,4,*(), 蔡勇1,3, 江桂斌1,2,4   

  1. 1 中国科学院生态环境研究中心 北京 100085
    2 中国科学院大学 北京 100049
    3 佛罗里达国际大学化学与生物化学系 美国迈阿密 33199
    4 国科大杭州高等研究院环境学院 杭州 310000
  • 收稿日期:2020-09-29 修回日期:2020-11-26 出版日期:2021-01-24 发布日期:2020-12-09
  • 通讯作者: 阴永光
  • 作者简介:
    * Corresponding author e-mail:
  • 基金资助:
    国家自然科学基金项目(21976193); 中科院前沿科学重点研究计划(QYZDB-SSWDQC018); 中科院创新交叉团队(JCTD-2018-04); 万人计划青年拔尖人才(W03070030); 中科院青年创新促进会(2016037)
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Analysis Methods, Occurrence, and Transformation of Reactive Gaseous Mercury in the Atmosphere

Yingying Fang1,2, Ying Wang1,2, Jianbo Shi1,2,4, Yongguang Yin1,2,4,*(), Yong Cai1,3, Guibin Jiang1,2,4   

  1. 1 Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences,Beijing 100085, China
    2 University of Chinese Academy of Sciences,Beijing 100049, China
    3 Department of Chemistry and Biochemistry, Florida International University, Miami, Florida 33199, United States
    4 School of Environment, Hangzhou Institute for Advanced Study, University of Chinese Academy of Sciences,Hangzhou 310000, China
  • Received:2020-09-29 Revised:2020-11-26 Online:2021-01-24 Published:2020-12-09
  • Contact: Yongguang Yin
  • Supported by:
    the National Natural Science Foundation of China(21976193); the National Natural Science Foundation of China(QYZDB-SSWDQC018); the CAS Interdisciplinary Innovation Team(JCTD-2018-04); the National Young Top-Notch Talents(W03070030); the Youth Innovation Promotion Association of CAS(2016037)

活性气态汞(Reactive gaseous mercury, RGM),在大气环境中通常被认为是气态的氧化汞,主导大气汞沉降过程,对汞的全球循环至关重要。本文详细介绍了RGM的多种采样和分析方法,讨论并比较了当前技术的优势和局限性;对RGM在大气中的生成、赋存、清除等环境过程以及相关的机制进行了梳理,并探究各过程在大气汞循环过程中的贡献。针对当前RGM分析的难点(如赋存浓度低、采集困难)与关键科学问题(如赋存形态与转化),需着力发展实际环境中RGM采集和形态分析的可行方法,进而深入探究其环境行为。大气中RGM的分析方法和环境行为研究是极具挑战性的任务,将是未来大气汞研究的重要内容之一,对于深入理解RGM在大气汞循环过程中的作用具有重要的意义。

关键词： 活性气态汞, 采样, 分析, 形态, 赋存, 清除

Reactive gaseous mercury(RGM), also known as gaseous oxidized mercury, dominates atmospheric mercury deposition and is critical to the global cycle of mercury. This review introduces various sampling and analysis methods of RGM in detail, and discusses the advantages and limitations of the current techniques. The environmental processes including the formation, occurrence, and depletion of RGM in the atmosphere and related mechanisms are reviewed, and the contribution of each process in the atmospheric mercury cycle is explored. In view of the current analytical difficulties of RGM(e.g., ultralow concentration and sampling problems) and key scientific issues(e.g., chemical form and transformation) in the RGM research, efforts should be made to develop the feasible methods for RGM collection and speciation determinatiton in the real environment, so as to further explore its environmental behavior. This is challenging but important for the research of atmospheric mercury and will be helpful for understanding the role of RGM in cycle processes of atmospheric mercury.

Contents

1 Introduction

2 Sampling and analysis of reactive gaseous mercury

2.1 Sampling of reactive gaseous mercury

2.2 Analysis of reactive gaseous mercury

3 Occurrence and transformation of reactive gaseous mercury in the atmosphere

3.1 Formation of reactive gaseous mercury in the atmosphere

3.2 Occurrence of reactive gaseous mercury in the atmosphere

3.3 Depletion of reactive gaseous mercury from the atmosphere

4 Conclusion and outlook

Key words: reactive gaseous mercury, sampling, analysis, chemical species, occurrence, depletion
()
图1 三种活性气态汞采样方法示意图 (a)镀KCl扩散管法[20]、(b)多级滤膜法[21]和(c)回流喷雾箱法[22](根据文献[20]、[21]、[22]重绘)
Fig. 1 Three sampling methods of reactive gaseous mercury (a) KCl-coated denuder[20],(b )Multi-membrane filter[21] and(c) Mist chamber[22](modified from reference [20]; [21]; [22])
表1 活性气态汞采集和分析方法的比较
Table 1 Comparison of sampling and analysis of reactive gaseous mercury
Sampling methods Material types Analysis Speciation Time Flow rate
(L·min-1)		 LOD
(pg·m-3)		 Application Comments ref
KCl-coated denuder KCl Acid rinse, SnCl2-CVAFS/Thermal desorption, CVAFS Total RGM 1~12 h 10 0.5~6.2 Tekran?
1130		 Automated, easy operation 20
Multi-membrane filter CEM Acid digestion, SnCl2-CVAFS Total RGM 2 w NA 0.02~
0.19a		 Aerohead plate Passive, easy
operation		 26
2 w NA 5 Box sampler Passive, easy
operation		 27
2 w 1 15 UNR-RMAS Manual, easy
operation		 28
Nylon membrane Temperature programmed desorption, CVAFS Total RGM, and
possible species
(HgBr2, HgCl2,
HgSO4, HgO,
Hg(NO3)2)		 2 w 1 NA UNR-RMAS Manual, species identification 28
Mist chamber HCl/NaCl SnCl2-CVAFS Total RGM 1 h 15~20 4 NA Manual, complicated operation 29
Others MnO2 sorbent Solvent trapping,
injection, GC-MS		 Hg(NO3)2 1 h NA NA NA Species identification 30
Particle-based sorbent trap Thermal desorption, APCI-MS HgBr2, HgCl2 24 h ~1 4~11 NA Species identification 31
表2 不同采样方法活性气态汞观测结果的比较
Table 2 Comparison of reactive gaseous mercury monitoring results by different sampling methods
Year Sampling methods RGM
(pg·m-3)		 Flow rate
(L·min-1)
(Sampling time)		 Blank MDL ref
1998 Mist chamber with 0.1 M HCl 16 12(23 h) NA NA 9
Tubular KCl-coated denuders 22±3 1(23 h) NA NA
Annular KCl-coated denuders 14.1 5(23 h) NA NA
1999 Multistage filter packs 54.2 3~5(6、24 h) NA 7 pg 44
Refluxing mist chambers 16.9 10(75~120 min) NA 5 pg
KCl-coated denuders 44.4 10(100~120 min) NA 15 pg
2011 KCl-coated denuders 13.6 4(1 h) <5 pg·m-3 <5 pg·m-3 34
Cation exchange membranes 38.3 1(2 w) 310±230 pg NA
Nylon membranes 25.6 1(2 w) 20±40 pg NA
2014 Tekran?1130 22.3±4.7 7(1 h) NA NA 28
UNR-RMAS(cation exchange membrane) 82.5±30.0 1(1~2 w) 0.2±0.3 ng(n=96) 0.3 ng
UNR-RMAS(nylon membrane) 14.2±10.3 1(1~2 w) 0.006±0.02 ng
(n=80)		 0.006 ng
2019 Tekran?1130 3 5.5(2 h) NA NA 35
UNR-DCS(cation exchange membrane) 20 2(1 w) NA 40 pg
UNR-RMAS(cation exchange membrane) 49 1(1 w) NA 40 pg
UNR-RMAS(nylon membrane) 8 1(1 w) NA 40 pg
2014 Tekran?1130 2.0±3.6 10(1 h) NA 1.5 pg·m-3 37
UNR-RMAS(cation exchange membrane) 24±15 1(2 w) 0.37±0.26 ng
(n=77)		 2~68 pg·m-3
UNR-RMAS(nylon membrane) 0.6±0.5 1(2 w) 0.03±0.03 ng
(n=69)		 0.01~14.6
pg·m-3
2017 KCl-coated denuder 9.92±17.44 ~1(3 h) 27.6±2.9 pg(n=11) 3 pg 40
KCl-coated glass fiber filter 87.25±101.29 ~1(3 h) 57.3±5.2 pg(n=11) 3 pg
KCl-coated quartz sand tube 203.75±139.09 ~1(3 h) 29.8±4.5 pg(n=11) 3 pg
Cation exchange membrane 264.78±130.19 ~1(3 h) 79.8±9.5 pg(n=8) 3 pg
图2 不同汞化合物 (a)和野外样品(b~g)的程序升温热解析图谱。通过比对野外样品和汞标准品的程序升温热解析图谱,推断野外样品中汞的形态。(b)HgCl2、HgBr2;(c)Hg-S和Hg-N类化合物;(d)汞的混合物;(e)HgO、Hg-N和Hg-S类化合物;(f)Hg-N类以及峰出现高拖尾的未知化合物;(g)峰值逐渐升高的未知化合物[28]
Fig. 2 Temperature programmed desorption profiles of different Hg compounds (a) and field samples(b~g). By comparing temperature programmed desorption profiles of field sample to those of mercury standard, the Hg species in field samples could be inferred;(b) shows HgCl2/HgBr2;(c) shows Hg-sulfur, and nitrogen compounds;(d) shows a mixture of compounds;(e) shows HgO, Hg-nitrogen, and sulfur compounds;(f) shows Hg-nitrogen compounds with an unknown compound producing a high residual tail, and(g) shows a gradual increase with an unknown peak[28]. Copyright 2016, American Chemical Society
图3 大气汞的化学转化过程图
Fig. 3 Chemical transformation of mercury in the atmosphere
表3 国内外不同地点的活性气态汞浓度对比
Table 3 Comparison of reactive gaseous mercury from worldwide locations
Continent Site Region Type Period RGM(pg·m-3) ref
Northern Hemisphere
Asia Beijing North China Urban 2015~2016 18.47±22.27 74
Miyun North China Remote 12/2008~11/2009 10.1±18.8 75
Ningbo Yangtze River Delta Urban 7/2013~1/2014 197±246 76
Guiyang Southwest China Urban 8~12/2009 35.7±43.9 77
Xiamen Southeast China Coastal 3/2012~2/2013 61.05±69.41 78
Chongming East China Coastal 2009~2012 8.0±8.8 79
Taoyuan Taiwan, China Remote 10/2017~9/2018 12.1±34.3 80
Bohai Sea/Yellow Sea Northeast China Sea Spring/2014 2.5±1.7 81
Fall/2014 4.3±2.5
South China Sea South China Sea 9/2015 6.1±5.8 82
Mt. Changbai Northeast China Mountain 7/2013~7/2014 5.4±6.4 83
Mt. Waliguan Northwest China Mountain 9/2007~9/2008 7.4±4.8 84
North America Nevada Reno Urban 2/2007~1/2009 18±22 85
Michigan Detroit Urban 2004 15.5±54.9 86
Dexter Rural 2004 3.8±6.6
Canada Toronto Remote 12/2003~11/2004 14.2±13.2 87
Mexico Mexico City Urban 3/2006 62±64 88
Oregon, U.S.A. Mt. Bachelor Mountain 5~8/2005 43 89
Colorado, U.S.A. Mt. Rocky Mountain 4~7/2008 20 90
Alaska, U.S.A. Beaufort Sea Sea ice 3~4/2009 30.1 91
Europe Mediterranean Sea - Coastal/Sea Summer/2015 11.8±15.0 92
Southern Hemisphere
Amsterdam Island - Ocean 1/2012~12/2013 0.34 93
Africa South Africa - Ocean 10/2006 3.4±4 94
表4 活性气态汞的不同清除方式及其影响因素
Table 4 Different depletion ways of reactive gaseous mercury and the influencing factors
Depletion ways RGM behaviors Influencing factors
Deposit to
land surface		 Dry deposition RGM species
Environmental conditions
Land surface types
Gas-liquid partition Wet deposition RGM species
Temperature
Precipitation types
Gas-particle partition Transform to PBM RGM species
Temperature
Aerosol compositions
Photochemical reduction Transform to GEM RGM species
Solar radiation
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