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Progress in Chemistry 2021, Vol. 33 Issue (9): 1627-1647 DOI: 10.7536/PC200836 Previous Articles   Next Articles

• Review •

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: Revised: Online: Published:
  • Contact: Chungang Yuan
  • Supported by:
    National Natural Science Foundation of China(91543107); Fundamental Research Funds for the Central Universities(2017ZZD07)
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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
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
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
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
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
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
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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