| 上海城区多环芳烃及其衍生物的污染特征与健康风险评估 |
| 摘要点击 1140 全文点击 163 投稿时间：2024-03-11 修订日期：2024-05-03 |
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| 中文关键词 细颗粒物 硝基多环芳烃（NPAHs） 含氧多环芳烃（OPAHs） 二维气相色谱-飞行时间质谱（GC×GC-ToF-MS） 来源 健康风险评估 |
| 英文关键词 PM2.5 nitrated polycyclic aromatic hydrocarbons （NPAHs） oxygenated polycyclic aromatic hydrocarbons （OPAHs） two-dimensional gas chromatography time-of-flight mass spectrometry （GC×GC-ToF-MS） sources health risk assessment |
| 作者 | 单位 | E-mail | | 涂炯 | 广西大学化学化工学院, 南宁 530004
上海市环境科学研究院生态环境部城市大气复合污染成因与防治重点实验室, 上海 200233 | 15706162659@163.com | | 马英歌 | 上海市环境科学研究院生态环境部城市大气复合污染成因与防治重点实验室, 上海 200233 | mayg@saes.sh.cn | | 戴海夏 | 上海市环境科学研究院生态环境部城市大气复合污染成因与防治重点实验室, 上海 200233 | | | 冯馨蔚 | 上海市环境科学研究院生态环境部城市大气复合污染成因与防治重点实验室, 上海 200233 | | | 吴宇航 | 上海市环境科学研究院生态环境部城市大气复合污染成因与防治重点实验室, 上海 200233 | | | 狄睿苗 | 上海市环境科学研究院生态环境部城市大气复合污染成因与防治重点实验室, 上海 200233 | | | 乔利平 | 上海市环境科学研究院生态环境部城市大气复合污染成因与防治重点实验室, 上海 200233 | | | 周敏 | 上海市环境科学研究院生态环境部城市大气复合污染成因与防治重点实验室, 上海 200233 | | | 童张法 | 广西大学化学化工学院, 南宁 530004 | zhftong@sina.com |
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| 中文摘要 |
| 多环芳烃（PAHs）及其衍生物硝基多环芳烃（NPAHs）和含氧多环芳烃（OPAHs）因其突出的诱变性和致癌性不断地受到人们的关注. 使用大流量采样器采集2022~2023年上海城区冬、夏季大气细颗粒物（PM2.5）的昼夜样品,采用二维气相色谱-飞行时间质谱（GC×GC-ToF-MS）定量PM2.5中的PAHs、NPAHs和OPAHs,对其昼夜质量浓度变化、来源和健康风险进行分析和评估. 结果表明,冬季ρ（PAHs）、 ρ（NPAHs）和ρ（OPAHs）的日均值分别为4.44、0.89和2.38 ng·m-3,夏季质量浓度水平低于冬季,分别为0.20、0.04和0.40 ng·m-3. 细颗粒物PM2.5中NPAHs质量浓度比PAHs和OPAHs质量浓度低1~2个数量级. 夏季PAHs和NPAHs中的物质质量浓度表现为白天高于夜晚,白天各物质质量浓度相较于夜晚增加-19.6%~193.6%,OPAHs则相反；冬季样品中大多数物质质量浓度则表现为夜晚高于白天. PAHs中在采样期间质量浓度最高的物质是荧蒽和苯并[b]荧蒽,NPAHs和OPAHs在采样期间质量浓度最高的物质分别是9-硝基蒽和蒽醌. 基于相关性分析和特征比值法来源分析的结果,上海城区PM2.5中PAHs及其衍生物受车辆排放和煤炭、生物质燃烧的混合排放源的影响. PAHs和NPAHs的主要来源是交通,OPAHs多来自和PAHs相同的一次排放源. 与夏季相比,冬季的一次排放对大气中PAHs及其衍生物生成影响更大. 通过比较采样期间PM2.5中PAHs、NPAHs和OPAHs在冬、夏的毒性当量发现,冬季TEQ的日均值（441.4 pg·m-3）高于夏季（39.8 pg·m-3）10倍多,夜晚的TEQ高于白天. 潜在致癌风险大多来源于PAHs,NPAHs和OPAHs引起的ILCR值比PAHs低1~2个数量级. 根据终生致癌风险增量模型计算的健康风险评估结果显示,成人的总致癌风险高于青少年和儿童,女性通过不同暴露途径产生的致癌风险比男性更高. 成人因呼吸吸入和皮肤接触而患癌症的风险高于青少年和儿童,而青少年因口服摄入而患癌症的风险更高. 结果显示,上海城区冬、夏季大气细颗粒物中PAHs及其衍生物的致癌风险在可控范围. |
| 英文摘要 |
| Polycyclic aromatic hydrocarbons （PAHs） and their derivatives, nitrated polycyclic aromatic hydrocarbons （NPAHs） and oxygenated polycyclic aromatic hydrocarbons （OPAHs）, have been under constant scrutiny for their prominent carcinogenicity and mutagenicity. In this study, fine particulate matter （PM2.5） was collected in the urban area of Shanghai from 2022 to 2023. Their diurnal and nocturnal mass concentration variations, sources, and health risk assessment were analyzed. Two-dimensional gas chromatography-time-of-flight mass spectrometry （GC×GC-ToF-MS） was used to quantify PAHs, NPAHs, and OPAHs. The results showed that the daily average concentrations of PAHs, NPAHs, and OPAHs were 4.44, 0.89, and 2.38 ng·m-3, respectively, in winter. The concentration levels were much lower in summer than those in winter, which were 0.20, 0.04, and 0.40 ng·m-3, respectively. The ratio of the concentrations of NPAHs to those of PAHs and OPAHs concentrations by 1-2 orders of magnitude. The substance concentrations of PAHs and NPAHs in summer were higher in the daytime than those at nighttime and vice versa for OPAHs. Concentrations of the few target substances in winter samples were higher at night. The substances with the highest concentrations of PAHs during the sampling period were fluoranthene and benzo（b）fluoranthene, whereas the substances with the highest concentrations of NPAHs and OPAHs were 9-nitroanthracene and 9,10-anthraquinone, respectively. Based on the results of correlation analysis and source analysis by the diagnostic ratios, PAHs and their derivatives in PM2.5 in the urban area of Shanghai were affected by mixed emission sources, with primary emissions accounting for a significant portion. In addition to vehicle emissions and some coal and biomass combustion, the generation of PAHs was also affected by aerosol aging. Vehicle emissions were the major source of NPAHs, whereas OPAHs might be from the same primary emission sources as those of PAHs. Primary emissions contributed more to PAHs in winter than in summer. Comparison of the toxic equivalents of PAHs, NPAHs, and OPAHs in PM2.5 in winter and summer during the sampling period revealed that the average daily TEQ value was higher in winter （441.4 pg·m-3） than that in summer （39.8 pg·m-3）, which was consistent with the seasonal variation of mass concentrations. The toxicity of PAHs and their derivatives in PM2.5 in the Shanghai urban area was higher during nighttime than that in the daytime. Most of the potential carcinogenic risk originated from PAHs, and the ILCR values caused by NPAHs and OPAHs were 1-2 orders of magnitude lower than those caused by PAHs. The results of health risk assessment based on incremental lifetime cancer risk modeling showed that the total cancer risk was higher in adults than that in adolescents and children and that females had a higher cancer risk than males through different exposure pathways. Adults had a higher risk of cancer from respiratory inhalation and dermal exposure than that of adolescents and children, whereas adolescents had a higher risk of cancer from oral ingestion. The results showed that the carcinogenic risk of PAHs and their derivatives in the atmosphere in the urban area of Shanghai in winter and summer was within controllable range. |
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