Study on the Characteristics of Heavy Metal Contents and Annual Fluxes of Atmospheric Dry and Wet Deposition in Jinan City Using AFS and ICP-MS
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摘要:
大气降尘是地表土壤重金属元素的重要来源, 研究大气降尘中重金属元素的地球化学特征并进行源解析对制定污染防控政策具有重要的指导作用。本文采用原子荧光光谱法、电感耦合等离子体质谱法、X射线荧光光谱法分析济南市大气干湿沉降中8种重金属(砷镉铬铜汞镍铅锌)含量特征; 采用相关分析及主成分分析方法对大气干湿沉降重金属进行源解析。结果表明, 大气干湿沉降物中镉铬铜汞镍铅锌平均含量分别为2.07 mg/kg、135.9 mg/kg、65.7 mg/kg、218.6 μg/kg、110.7 mg/kg、380 mg/kg, 显著高于土壤背景值, 且富集程度高, 明显受人为活动污染。镉铜汞铅主要来源于燃煤, 砷铬来源于道路尘, 镍来源于土壤, 锌来源于交通尘; 燃煤和道路尘对大气降尘的贡献率为50.13%, 两者是济南市大气降尘污染的主要来源。大气干湿沉降对城区表层土壤中镉汞铬铅锌及砷的含量水平影响显著, 其中锌年沉降通量最高(均值148 mg·m-2·a-1), 汞年沉降通量最低(均值0.085 mg·m-2·a-1), 且镉汞含量增长速率较高; 大气干湿沉降对砷铬在土壤中的累积影响显著。
Abstract:Atmospheric deposition is an important source of heavy metals in surface soil, the study on the geochemical characteristics and source analysis of heavy metals in atmospheric dust would provide important guidance for pollution prevention. The contents of heavy metals (As, Cd, Cr, Cu, Hg, Ni, Pb, Zn) in atmospheric dust in Jinan have been analyzed by Atomic Fluorescence Spectrometry (AFS), Inductively Coupled Plasma-Mass Spectrometry (ICP-MS), and X-ray Fluorescence Spectrometry (XRF). The correction analysis and principal components analysis (PCA) were used to source the heavy metals. The average contents of Cd, Cr, Cu, Hg, Pb and Zn in atmospheric dry and wet deposition are 2.07 mg/kg, 135.9 mg/kg, 65.7 mg/kg, 218.6 μg/kg, 110.7 mg/kg, 380 mg/kg, respectively, which are higher than the background values of these elements in soil and has an obvious enrichment due to the contamination by human activities. Cd, Cu, Hg, Pb are mainly derived from coal combustion, As and Cr are derived from road dust, Ni may be derived from soil dust, and Zn is derived from traffic discharges. The coal combustion and road dust are the main pollution sources of atmospheric deposition in Jinan, with the contribution proportion of atmospheric deposition up to 50.13%. Atmospheric dry and wet deposition produce significant effect on the contents of Cd, Hg, Cr, Pb, Zn and As in urban topsoil, the annual deposition flux of Zn is the highest with a mean of 148 mg/(m2·a), whereas the annual deposition flux of Hg is the lowest with a mean of 0.085 mg/(m2·a). Moreover, Cd and Hg contents have higher growth rates, and dry and wet atmospheric deposition significantly influences the As and Cr accumulation in soils.
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表 1 济南市大气干湿沉降重金属含量参数统计
Table 1. Parametric statistics of heavy metal elements contamination in dry and wet atmospheric deposition of Jinan City
含量指标 As Cd Cr Cu Hg Ni Pb Zn 含量指标 As Cd Cr Cu Hg Ni Pb Zn 最小值 3.62 0.9 35.17 27.15 82 13.49 46.14 115 最大值 35.02 3.96 3126 156.6 1165 114.9 235.2 1645 平均值 9.45 2.07 135.9 65.7 218.6 31.4 110.7 380 标准差 4.90 0.67 351.3 26.2 146.7 12.7 36.6 245 变异系数 0.50 0.32 2.58 0.40 0.67 0.40 0.33 0.64 富集系数 1.02 24.64 2.06 2.73 11.5 1.22 4.29 5.98 土壤背景值[15] 9.3 0.084 66.0 24.0 19 25.8 25.8 63.5 注：Hg含量单位为μg/kg，其他元素为mg/kg，样本数为78。 
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表 2 济南市大气干湿沉降重金属元素主成分分析
Table 2. Analytical results of PCA for dry and wet atmospheric deposition of Jinan City
元素 F1 F2 F3 F4 As 0.322 0.826 0.074 -0.107 Cd 0.690 -0.255 0.481 -0.169 Cr 0.071 0.913 0.141 0.090 Cu 0.677 0.259 -0.093 0.216 Hg 0.686 0.133 -0.007 0.152 Ni 0.042 0.232 0.896 0.143 Pb 0.835 0.212 0.158 -0.012 Zn 0.151 -0.092 0.109 0.932 特征值 2.24 1.77 1.11 0.99 方差贡献率(%) 27.96 22.17 13.82 12.48 累积贡献率(%) 27.96 50.13 63.95 76.43
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表 3 济南市大气干湿沉降重金属元素的年沉降通量
Table 3. Deposition flux of heavy metal elements in dry and wet atmospheric deposition of Jinan City
项目 年沉降通量(mg·m-2·a-1) 沉降物总量
(g·m-2·a-1)As Cd Cr Cu Hg Ni Pb Zn 最小值 0.67 0.21 8.0 5.6 0.016 3.36 12.6 33 125 最大值 21.79 5.05 1374.6 86.5 0.333 57.89 174.2 718 1668 平均值 4.53 0.85 57.8 26.4 0.085 12.47 43.3 148 406 标准差 3.78 0.63 156.2 14.6 0.058 7.64 25.7 103 252 变异系数 0.83 0.73 2.70 0.55 0.69 0.61 0.59 0.69 0.57
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