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化学进展 2021, Vol. 33 Issue (9): 1627-1647 DOI: 10.7536/PC200836 前一篇   后一篇

• 综述 •

大气颗粒物重金属形态分析

何安恩1,2,3, 解姣姣1, 苑春刚1,*()   

  1. 1 华北电力大学环境科学与工程系 保定 071000
    2 中国科学院生态环境研究中心 北京 100085
    3 中国科学院大学资源与环境学院 北京 100049
  • 收稿日期:2020-08-17 修回日期:2020-11-16 出版日期:2021-09-20 发布日期:2020-12-28
  • 通讯作者: 苑春刚
  • 基金资助:
    国家自然科学基金项目(91543107); 中央高校基本科研业务费项目(2017ZZD07)
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Heavy Metal Speciation Analysis and Distribution Characteristics in Atmospheric Particulate Matters

Anen He1,2,3, Jiaojiao Xie1, Chungang Yuan1()   

  1. 1 Department of Environmental Science & Engineering, North China Electric Power University, Baoding 071000, China
    2 Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China
    3 College of Resources and Environment, University of Chinese Academy of Sciences, Beijing 100049, China
  • Received:2020-08-17 Revised:2020-11-16 Online:2021-09-20 Published:2020-12-28
  • Contact: Chungang Yuan
  • Supported by:
    National Natural Science Foundation of China(91543107); Fundamental Research Funds for the Central Universities(2017ZZD07)

重金属作为大气颗粒物中重要有毒组分之一,其总量和存在形态与颗粒物重金属的健康风险密切相关。因此,颗粒物重金属形态分析对深入研究大气污染健康效应具有非常重要的意义。本文从以下四个方面对近年来国内外相关研究进行了归纳总结:(1)模拟体液、BCR、Tessier、Chester等逐级顺序提取方法被广泛用于重金属操作定义形态分析;(2)色谱-质谱联用技术和新型功能化材料用于重金属形态选择分析以及X射线吸收精细结构谱(XAFS)原位形态表征技术可以获取重金属价态、化合态、原子簇结构信息;(3)重金属形态粒径分布特征复杂,受多种因素影响,倾向于富集在细颗粒物中;(4)重金属形态时空分布具有很强的区域性,社会发展、工业来源、气候条件是主要影响因素,夏冬季节和雾霾天气危害性较大。

关键词： 颗粒物, 重金属, 形态分析, 生物有效性

Heavy metals (HMs), as one of the important toxic components in atmospheric particulate matters (PMs), are closely related to human health. The health risk of HMs in particulate matters highly depends on their species and bioavailability. Heavy metal speciation analysis in PMs is significant for the study of air pollution environmental health. Based on related researches in recent years, this paper summarizes and discusses about HMs species in atmospheric particulate matters from four key aspects: (1) Synthetic body fluids and sequential extraction procedures (such as BCR, Tessier's, Chester) have been widely used to extract operationally-defined species of HMs; (2) Chromatography-mass spectrometry technology and new functional materials have been applied for specific-selective analysis, and in-situ speciation and atomic cluster structures of HMs can be characterized by XAFS (X-ray absorption fine structure); (3) Particle size distribution of HMs species in PMs is complicated, which is affected by many factors and tends to be concentrated in fine particles; (4) Spatial and temporal distribution characteristics of HMs in PMs are highly regional. Social development, industrial, and climate are the main factors. Health risks at summer and hazy days are relatively higher.

Contents

1 Introduction

2 Heavy metal speciation analysis methods

2.1 Operationally-define speciation

2.2 Specific-selective speciation

2.3 In-situ speciation

3 Heavy metal speciation distribution characteristics

3.1 Spatial distribution characteristics

3.2 Temporal distribution characteristics

3.3 Particle size distribution characteristics

4 Conclusion and outlook

Key words: particulate matters, heavy metal, speciation, bioavailability
()
表1 国内外用于提取大气颗粒物可溶态重金属的提取剂及其化学组成
Table 1 Extractant and its chemical components for extracting soluble heavy metals from atmospheric particulate matters
Extractant Chemical components Reaction condition ref
Water Deionized water (pH=7.0) Shake/ultrasonicate for several hours 43⇓⇓⇓⇓⇓~49
Buffered salt solution/dilute acid Normal saline (0.9% NaCl solution, pH=7.0)
1 mM Ethylenediaminetetraacetic acid (EDTA, pH=4.77)
10 mM CH3COOK/CH3COOH (acetate buffer, pH=4.3)
6∶2∶5 v/v HNO3∶HCl∶HClO4 (pH=1.0)
0.4% v/v HNO3 solution (pH=1.2)
15 mL 0.1 mol/L HCl (pH=1.0)		 Ultrasonicate for 30 mins
Ultrasonicate for 15 mins
Ultrasonicate for 15 mins
Shake at 95 ℃ for 4 h
Shake for 24 h
Shake for 1 h		 50
49
49
51
52
53
Serum-based fluid 4.5 g/L contained glucose, 2.4 g/L HEPES(4-(2-hydroxyethyl)-1-piperazineethanesulfonic acid), 1500 g/L NaHCO3, 0.11 g/L Na-pyruvate,0.29 g/L L-glutamine,5 mL penicillin/streptomycin, 50 mL fetal bovine serum. (pH=7.4) Slowly shake at 37 ℃ for 24 h 54
Physiologically based
extraction test (PBET)-simulated gastric juice		 0.5 g sodium citrate, 0.5 g malic acid, 420 μL lactic acid, 500 μL acetic acid, 1.25 g pepsin, finally dilute the volume to 1L with deionized water. (adjust pH to 2.0 with NaOH and HCl) Slowly shake at 37 ℃ for 24 h 55,56
Physiologically based
extraction test (PBET)-simulated intestinal
juice		 0.5 g sodium citrate, 0.5 g malic acid, 420 μL lactic acid, 500 μL acetic acid, 1.25 g pepsin, 0.05 g trypsin, 0.175 g bile salts, finally dilute the volume to 1L with deionized water. (adjust pH to 7.0 with saturated NaHCO3) Slowly shake at 37 ℃ for 24 h 55,56
Surrogate lung fluid
(SLF)		 130 mM NaCl, 5 mM KCl, 1.2 mM MgSO4, 5mM NaHCO3, 1.5 mM CaCl2, 5.5 mM glucose, 10 mM HEPES. (pH=7.4) Slowly shake in the dark at
37 ℃		 57⇓~59
Artificial lysosomal fluid (ALF) 0.05 g/L MgCl2, 3.21 g/L NaCl, 0.071 g/L Na2HPO4, 0.039 g/L Na2SO4, 0.128 g/L CaCl2·H2O, 0.077 g/L C6H5Na3O7·2H2O, 6.00 g/L NaOH, 20.8 g/L C6H8O7, 0.059 g/L NH2CH2COOH, 0.090 g/L C4H4O6Na2·2H2O, 0.085 g/L C3H5NaO3, 0.086 g/L C3H3O3Na. (pH=4.5) Slowly shake in the dark at
37 ℃ in a closed container		 60,61
Gamble's solution 0.095 g/L MgCl2, 6.019 g/L NaCl, 0.298 g/L KCl, 0.126 g/L Na2HPO4, 0.063 g/L Na2SO4, 0.368 g/L CaCl2·H2O, 0.574 g/L C2H3O2Na, 2.604 g/L NaHCO3, 0.097 g/L C6H5Na3O7·2H2O. (pH=7.4) Slowly shake in the dark at 37 ℃ in a closed container 60,61
表2 文献中主要的逐级提取法及其应用
Table 2 The main sequential extraction procedure in the literature and their applications
Procedure's
name		 Year of
proposal		 0: Water-
soluble fraction		 1: Exchangeable fraction 2: Acid-soluble fraction
(carbonate bound)		 3: Reducible fraction
(Fe-Mn oxide bound)		 4: Organic, oxidative and
sulphides fraction		 5: Residual fraction ref/applications
Tessier 1979 - MgCl2 or CH3COONa CH3COONa+CH3COOH Na2S2O4+sodium citrate+citric acid or
NH2OH·HCl+25%(v/v)
CH3COOH		 HNO3+H2O2+CH3COONH4 HF+HClO4 74/81, 82
M1-Tessier 1986 1% NaCl NH2OH·HCl+
25%(v/v)
CH3COONH4		 - HNO3+H2O2+CH3COONH4 HNO3+HCl+H2O 77/83, 84
M2-Tessierα 1989 - MgCl2 20~80 mL 20~80 mL 20~80 mL HF+HClO4 78/85, 86
M3-Tessier 1992 CH3COOH or
CH3COONH4		 HCl+NH2OH·HCl H2C2O4+(NH4)2C2O4 HNO3+H2O2 6 mol/L HCl 79/87, 88
M4-Tessier 2005 H2O MgCl2 CH3COOH/CH3COONa NH2OH·HCl+25%(v/v)
CH3COOH		 H2O2+HNO3+CH3COONH4 - 80/89, 90
Chester 1989 - CH3COONH4 or
MgCl2		 “Chester-Hughes” reagentβ - “Chester-Hughes” reagentβ HNO3+HFc 91/92, 93
Sequential extraction procedure 1998 H2O 0.25 M
NH2OH·HCl		 H2O2+CH3COONH4 HNO3+HCl+HClO4 94/48, 95, 96
Five-step extraction procedure 2001 - (NH4)2SO4 NH4H2PO4 (NH4)2C2O4 (NH4)2C2O4+ascorbic acid HNO3+H2O2+HF 97/29, 98
BCR 1993 0.11 mol/L
CH3COOH		 0.1 mol/L
NH2OH·HCl		 8.8 M H2O2+1 M
CH3COONH4		 - 75/99, 100, 101
M-BCR 1998 - - CH3COOH NH2OH·HCl+HNO3 H2O2+CH3COONH4+HNO3 HNO3 102/28, 103
表3 中国、世界主要国家和地区的环境空气重金属标准限值(年均值,ng/m3)
Table 3 Standard limits for heavy metals in ambient air in China and major countries around the world (Annual mean, ng/m3)
Standard name Pb V As Mn Ni Cr Hg Cd ref
GB 3095—2012 500 - 6 - - 0.025 50 5 158
WHO 100 1000a 6.6b 150 25a 0.25b 1000 5 159
EU 500 - 6 - 20 - 5 160
USEPA 150c - 6 - 20 - - 161
表4 国外主要地区大气颗粒物重金属元素生物有效性平均体积浓度特征(ng/m3)
Table 4 The characteristics of the average volume concentration of heavy metal elements bioavailability in atmospheric particulate matters in foreign regions (ng/m3)
Region Cd Cr Cu Ni Pb Zn As Mn Fe Al V ref
Europe
Czech Republica 0.05~0.13 0.37~0.88 0.64~1.10 0.35~1.65 0.26~1.26 0.03~1.39 0.77~4.17 - - - - 169
Romania 0.159 - 4.412 0.884 1.919 6.944 - - - - - 57
Austria - <LOD-2.0 1.8~14.7 <LOD-2.6 - - - 1.6~32.4 8.6~260.6 - - 163
Poland 1.1 1.05 5.6 0.75 15.95 18.05 1.15 8.35 133.25 2.35 0.35 162
Asia
Pakistan 46.2 11.1 - 2.7 281.6 6380 - 93 - - - 164
Indonesia 3 161 67 89 59 99 - 87 819 137 - 184
India 1.187 4.283 91.1733 12.9167 22.113 76.36 - 6.21 469.59 - - 183
Africa
Nigeria - 10.75 0.438 - 4.05 - - - - 16.47 - 185
Egyptb 35 - - - 703 - - 756 3038 - - 165
America
United States 0.072 0.198 22.083 0.306 0.7399 17.22 - 2.294 19.3372 0.1703 - 166
Canadac - - 511.297 - 1574.6 2982.11 - 275.77 686.261 - 25.092 167
Oceania
New Zealand - - 19.5667 - 79.85 122.267 112.3 9.15 90.1 - 17.4 168
表5 中国各城市大气颗粒物重金属元素生物有效性平均体积浓度特征(ng/m3)
Table 5 The characteristics of the average volume concentration of heavy metal elements bioavailability in atmospheric particulate matters in Chinese cities (ng/m3)
Chinese city Cd Cr Cu Ni Pb Zn Fe As Al V Mn ref
East China
Hefeia 0.653 7.378 - 7.0772 41.0476 207.433 - - - 7.581 222.146 178
Nanjing 3.38 11.10 38.67 7.51 143.42 366.28 253.1 8.02 - - 48.82 179
Hangzhou - - - - 37.124 - - - - - - 180
Donghai 0.36 0.24 28.0 0.27 5.6 38.0 21.0 0.74 21.0 1.7 5.5 181
Shanghaib - - 17.2 - 15.4 98.933 - - - - 30.6 56
North China
Baoding 4.599 6.138 99.576 - 141.688 257 - 32.019 - - - 28,29
Beijing 3.5 3.4 36 28.6 96 851 200 19.5 138 2.2 52 186
Taiyuan 1.68 - - - 141.9 - - - - - - 187
South China
Guangzhou 4.183 1.199 34.015 2.293 188.305 498.1 249.935 14.985 200.95 - 40.06 84
Dongguan 4.48 17.148 111.024 100.152 126.728 1975.38 769.423 52.302 940 11.739 81.351 174
Macau 1.699 16.354 309.643 11.529 9.467 1322.27 - 7.506 - 6.536 - 175
Northeast China
Jinzhou 0.653 11.27 112.535 - 153.34 625.37 - - 360 - - 177
Southwest China
Guiyang 3.33 - 26.417 - 18.583 711.9167 399.167 406.33 2095.67 6.333 1483.5 176
表6 国内四个城市利用逐级提取法分析不同粒径重金属的形态平均百分比汇总表
Table 6 A summary table of the average percentage of heavy metals speciation with different particle sizes analyzed by the sequential extraction procedures in four domestic cities
City Baoding[216] Xiamen[217] Beijing[218] Nanjing[67]
Sequential extraction
procedure		 Five-step extraction procedure M-BCR M-Tessier M-BCR
Particle size PM2.5 PM10 TSP PM2.5 PM10 PM2.5 TSP PM2.5 TSP
As F1 % 45.475 37.34 29.76 5 2 52 31 44 49.5
F2 % 14.9925 13.975 12.8875 1 1 26 40 30.5 30.5
F3 % 12.4075 11.685 11.0025 3 2 15 16 6.5 5
F4 % 19.185 19.7375 18.0025 91 95 7 14 19 15
F5 % 7.94 17.2625 28.3475 - - - - - -
Cd F1 % - - - 75 52 34 39 59.5 57.5
F2 % - - - 4 11 13 36 9 9.5
F3 % - - - 13 12 42 16 10 5
F4 % - - - 8 25 11 9 21.5 28
Pb F1 % - - - 23 21 20 5 36.5 36
F2 % - - - 57 59 41 60 34 38.5
F3 % - - - 3 5 23 20 18.5 13.5
F4 % - - - 17 15 16 14 11 12
Ni F1 % - - - 56 36 4 17 7 15
F2 % - - - 7 14 65 18 21 16
F3 % - - - 15 12 25 54 47.5 34
F4 % - - - 22 38 6 11 24.5 35
Cu F1 % - - - 66 71 17 19 31.5 42.5
F2 % - - - 9 7 21 25 17 21.5
F3 % - - - 17 5 11 38 25 21.5
F4 % - - - 8 17 51 18 26.5 14.5
Zn F1 % - - - 56 63 20 41 57.5 60.5
F2 % - - - 5 6 30 35 11.5 15
F3 % - - - 4 8 27 19 20 13
F4 % - - - 35 23 23 6 11 11.5
Mn F1 % - - - 57 53 44 34 37.5 36.5
F2 % - - - 4 7 25 27 9 11
F3 % - - - 2 13 26 28 23 16
F4 % - - - 19 27 5 12 30.5 36.5
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摘要

大气颗粒物重金属形态分析