The Content Characteristics and Source Analysis of Polycyclic Aromatic Hydrocarbons in Topsoil of Beijing City
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摘要:
土壤，作为城市中最重要的环境介质，承担了较高多环芳烃（PAHs）的环境负荷，开展土壤PAHs分布特征及来源分析研究，可以为污染风险防控、环保政策制定提供支撑。为研究北京市不同功能区土壤环境中PAHs的含量、组成及来源，本文在北京市主城区进行了大范围采样，同时针对工业区、农业种植区、水源保护区及居民区等不同功能区进行了分区采样，共采集了表层土壤样品459份，采用气相色谱-质谱法（GC-MS）测定16种PAHs单体含量。结果表明：主城区3个分区（东南-中心-西北）表层土壤中16种PAHs总量的均值分别为153.7μg/kg、333.2μg/kg和142.9μg/kg。工业区3个分区（东南工厂、首钢工业、大台煤矿）表层土壤中16种PAHs总量的均值分别为1006.9μg/kg、1379.4μg/kg及146.8μg/kg。水源保护区2个分区（怀柔、密云）表层土壤中16种PAHs总量的均值分别为86.4μg/kg和154.5μg/kg。农业种植区4个分区（昌平、平谷、房山、通州）表层土壤中16种PAHs总量的均值分别为109.0μg/kg、118.3μg/kg、106.8μg/kg及94.2μg/kg。居民区中16种PAHs总量的均值为131.1μg/kg。与前人关于PAHs含量及分布特征的研究结果对比，北京市表层土壤中PAHs含量呈下降趋势，这与北京市近年来燃煤使用量下降及天然气使用量增加有关。不同功能区PAHs成分组成存在一定的差异，工业区重环和中环PAHs占比高，而水源保护区、农业种植区以及居民区的轻环占比总体上高于工业区，这是由于不同功能区PAHs的来源存在差异。主成分分析-多元线性回归法的分析结果表明：主城区PAHs的主要来源是尾气排放以及石油储存运输过程中泄漏，贡献率分别为81.46%和18.54%；工业区表层土壤中PAHs的主要来源有煤炭燃烧以及尾气排放，贡献率分别为62.65%和37.35%；居民区PAHs的主要来源由尾气排放源和天然气燃烧源组成，贡献率分别为53.30%和46.70%。进一步加强北京市交通管制，继续缩减煤炭在北京地区能源结构中的比重，增加清洁能源比重，是减少PAHs排放和污染的有效途径。
Abstract:BACKGROUND Polycyclic aromatic hydrocarbons (PAHs), as a typical persistent organic pollutant, widely exist in the environment and have high stability. Studying of the content distribution and source analysis of PAHs in soil will provide a technical basis for PAHs pollution prevention and control, ecological environment improvement and environmental protection policy-making.
OBJECTIVES In order to investigate the content, composition and source of PAHs in the soil environment of different functional areas in Beijing City.
METHODS A large-scale sampling was carried out in the core area of Beijing City. At the same time, regional sampling was carried out for different functional areas such as industrial areas, agricultural planting areas, water source protection areas and residential areas. A total of 459 topsoil samples were collected, and the monomer contents of 16 PAHs were analyzed by gas chromatography-mass spectrometry (GC-MS).
RESULTS The average values of the total contents of 16 PAHs (∑16PAHs) in topsoil of the three subregions in the core area (southeast, center and northwest) were 153.7, 333.2 and 142.9μg/kg, respectively. The average values of ∑16PAHs in topsoil of the industrial zone, including Southeast Factory, Shougang Industry and Datai Coal Mine, were 1006.9, 1379.4 and 146.8μg/kg, respectively. The average values of ∑16PAHs in topsoil of the water-conserving areas, Huairou and Miyun, were 86.4μg/kg and 154.5μg/kg, respectively. The average values of ∑16PAHs in topsoil of four agricultural planting regions (Changping, Pinggu, Fangshan and Tongzhou) were 109.0, 118.3, 106.8 and 94.2μg/kg, respectively. The average value of ∑16PAHs in topsoil of residential areas was 131.1μg/kg. Compared with previous research results on the content and distribution characteristics of PAHs, the content of PAHs in the topsoil in Beijing City showed a decreased trend, which was related to the decrease in the use of coal and the increase in the use of natural gas in Beijing City in recent years. The composition of PAHs in different functional areas was different. The proportion of heavy and medium rings PAHs were higher in industrial areas. The proportion of light rings PAHs in water-conserving areas, agricultural planting regions and residential areas was higher than that in industrial areas, which might be due to the different sources of PAHs in different functional areas. The results of principal component analysis-multiple linear regression method showed that the main sources of PAHs in the core area were tail gas emissions and leakage during oil storage and transportation, which contributed 81.46% and 18.54%, respectively. The main sources of PAHs in the topsoil of the industrial area were coal combustion and tail gas emissions, which contributed 62.65% and 37.35%, respectively. The main sources of PAHs in residential areas were tail gas emissions and natural gas combustion sources, with contribution rates of 53.30% and 46.70%, respectively.
CONCLUSIONS Further strengthening traffic control, continuing to reduce the proportion of coal in energy structure, and increasing the proportion of clean energy are effective ways to reduce PAHs emissions and pollution in Beijing City.
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表 1 北京市不同区域内表层土壤中多环芳烃含量统计
Table 1. Statistics of PAHs concentration in topsoil of different regions in Beijing City
北京市区域 样品数(件) 采样深度(cm) 所测PAHs单体数(种) PAHs总量范围(μg/kg) PAHs总量均值(μg/kg) 参考文献 居民区 31 0~5 16 219~27825 3917 Tang等(2005)[21] 四环外 47 5~30 16 14~4238 1056 Ma等(2005)[19] 四环内 30 5~30 16 467~5470 1637 Li等(2006)[18] 全市 138 0~10 15(萘除外) - 262.3 沈亚婷等(2008)[9] 五环内 233 0~10 16 93.3~13141.5 1228.1 Peng等(2011)[17] 六环内公园 122 0-10 16 66-6867 460 Qu等(2020)[20] 主城区 215 0~20 16 ND~2730.1 210.4 本文研究 工业区 57 0~20 16 ND~19466.5 1006.3 本文研究 居民区 44 0~20 16 ND~1407.1 131.1 本文研究 水源保护区 19 0~20 16 ND~399.4 118.6 本文研究 农业种植区 124 0~20 16 ND~456.8 106.9 本文研究 注：“-”代表无相应参考数据。 
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表 2 北京市表层土壤中PAHs主成分载荷及累积方差
Table 2. Component loading and cumulative variance of principal components for PAHs in topsoil of Beijing City
PAHs物质 主城区 工业区 居民区 PC1 PC2 PC1 PC2 PC1 PC2 萘 0.089 0.788 0.875 0.433 0.845 0.525 苊烯 0.229 0.858 0.265 0.918 0.855 0.517 苊 0.688 0.334 0.793 0.462 0.517 0.855 芴 0.841 0.211 0.294 0.888 0.517 0.855 菲 0.930 0.184 0.859 0.471 0.763 0.643 蒽 0.809 0.481 0.481 0.866 0.855 0.517 荧蒽 0.948 0.251 0.820 0.566 0.657 0.753 芘 0.940 0.258 0.759 0.632 0.625 0.778 苯并[a]蒽 0.973 0.175 0.462 0.885 0.654 0.745 䓛 0.974 0.183 0.931 0.351 0.512 0.847 苯并[b]荧蒽 0.964 0.214 0.944 0.323 0.864 0.474 苯并[k]荧蒽 0.979 0.176 0.318 0.944 0.579 0.808 苯并[a]芘 0.978 0.173 0.363 0.926 0.781 0.606 茚并[1, 2, 3-c, d]芘 0.969 0.189 0.449 0.882 0.824 0.552 二苯并[a, h]蒽 0.941 0.117 0.626 0.373 0.855 0.517 苯并[g, h, i]苝 0.913 0.193 0.383 0.920 0.763 0.621 方差(%) 74.63 13.53 58.17 35.35 59.35 39.56 累积方差(%) 74.63 88.16 58.17 93.52 59.35 98.91
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表 3 北京市表层土壤中PAHs多元线性回归分析的结果方程
Table 3. Resulting equations of multiple linear regression for PAHs in topsoil of Beijing City
北京市 Z R2 主城区 0.971PC1+0.221PC2 0.991 工业区 0.871PC1+0.487PC2 0.997 居民区 0.752PC1+0.659PC2 1.000
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表 4 北京市不同功能区表层土壤中PAHs多元线性回归方程
Table 4. Multiple linear regression equations for PAHs in topsoil of different functional areas in Beijing City
北京市 PAHs总量(∑16PAHs) 主城区 0.971σPAHPC1+0.221σPAHPC2+mean∑16PAHs 工业区 0.871σPAHPC1+0.487σPAHPC2+mean∑16PAHs 居民区 0.752σPAHPC1+0.659σPAHPC2+mean∑16PAHs 注：PCi代表了北京市不同功能区表层土壤中PAHs的不同来源；σPAH和mean∑16PAHs分别代表不同功能区表层土壤中16种PAHs单体总量的标准偏差和平均值。
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