| 滦河干流水体多环芳烃与有机氯农药季节性分布、组成及源解析 |
| 摘要点击 2402 全文点击 711 投稿时间：2017-03-13 修订日期：2017-04-19 |
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| 中文关键词 滦河 多环芳烃 有机氯农药 分布 组成 来源分析 |
| 英文关键词 Luanhe River polycyclic aromatic hydrocarbons organochlorine pesticides distribution composition source apportionment |
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| 中文摘要 |
| 为确定滦河水环境中多环芳烃（polycyclic aromatic hydrocarbons，PAHs）和有机氯农药（organochlorine pesticides，OCPs）的季节性分布、组成及来源，分别于2015年5月（春季）和8月（夏季）采集了滦河干流14个断面春、夏两季表层水体水样，采用GC-MS/MS分析了水体中17种PAHs和15种OCPs浓度.结果表明，滦河干流春季表层水体中PAHs总浓度范围是33.33~90.65 ng·L-1，平均值为52.64 ng·L-1；夏季PAHs总浓度范围是147.68~252.68 ng·L-1，平均值为169.88 ng·L-1；春季表层水体中OCPs总浓度范围是<0.08~3.48 ng·L-1，平均值为1.19 ng·L-1；夏季OCPs总浓度范围是<0.08~5.47 ng·L-1，平均值为1.02 ng·L-1.滦河干流春、夏两季表层水体中PAHs季节性污染特征表现为夏季PAHs总浓度高于春季，OCPs季节性污染特征整体表现为滦县、大黑汀水库坝上、潘家口村、郭家屯、曲家湾和白城子等6个断面春季OCPs总浓度低于夏季，其他8个监测断面则表现为春季要普遍高于夏季.从滦河春、夏两季表层水体PAHs和OCPs组成特征来看，春、夏两季PAHs以中低环为主且不同环数PAHs组成比例差异明显，其中春季主要以三环芳烃为主，其次是四环和二环，占PAHs总浓度的比例分别为51.18%~67.55%（平均为61.39%）、11.78%~33.94%（平均为20.97%）和13.31%~27.12%（平均为16.94%）；萘（Naphthalene，Nap）对滦河干流夏季表层水体中PAHs总浓度贡献最大，导致夏季PAHs以二环芳烃为主，占PAHs总浓度的比例为77.08%~90.62%（平均为83.34%），其次是三环芳烃和四环芳烃，分别占PAHs总浓度比例为7.09%~15.22%（平均为12.40%）和2.23%~7.49%（平均为3.97%）；春、夏两季表层水体中OCPs只有六六六（hexachlorocyclohexanes，HCHs）和滴滴涕（dichlorodiphenyltrichloroethanes，DDTs）有不同程度检出，且呈现以HCHs为主的污染特征，大部分断面HCHs主要组成部分是β-HCH，其中春季占HCHs总浓度的43.78%~70.09%，平均比例为56.25%；夏季占HCHs总浓度的53.63.00%~64.31%，平均比例为58.37%，其他断面则以α-HCH和γ-HCH为主要组成.分析滦河春、夏两季表层水体中PAHs和OCPs的来源，PAHs同分异构体比值显示滦河干流表层水体中PAHs主要来源于燃烧源，部分监测断面还存在石油源和混合源.OCPs同分异构体比值显示滦河干流春、夏两季表层水体中HCHs主要来源于环境残留和大气的长距离传输，另外春季乌龙矶和三道河子断面、夏季大黑汀水库坝上断面可能有新的林丹或γ-HCH输入；DDTs主要来源于新源输入和环境残留，其中潘家口水库坝上、三道河子、外沟门子、白城子、正蓝旗和闪电河水库等断面DDTs污染可能是由于新源输入，姜各庄和郭家屯断面DDTs主要来源于环境残留.滦河干流表层水体中除Chr浓度超过了美国国家水质标准外，其他各单体PAHs未超过各国或组织制定的水质标准，同时各单体PAHs也未超过不同国家或组织制定的水生生物暴露安全标准，但PAHs总浓度超过了美国环境质量标准和欧盟最大允许浓度规定的水生生物暴露安全限值，表明可能会通过水生生物富集PAHs对人类健康构成一定威胁；OCPs浓度不超过不同国家和组织制定的地表水水质标准，也不超过美国环保署制定的淡水水体水生生物水质基准，但春季姜各庄、乌龙矶、曲家湾和白城子及夏季潘家口水库坝上、潘家口村、曲家湾、白城子等断面α-HCH浓度超过其人体健康水质基准，春季闪电河水库断面p，p'-DDD浓度，以及姜各庄、三道河子、郭家屯和闪电河水库等断面p，p'-DDE浓度均超过了其人体健康水质基准，表明α-HCH、p，p'-DDD和p，p'-DDE对滦河干流这些断面周边居民健康会产生潜在有害影响. |
| 英文摘要 |
| Occurrence of 17 polycyclic aromatic hydrocarbons (PAHs) and 15 persistent organochlorine pesticides (OCPs) were analyzed by gas chromatography coupled to tandem mass spectrometry (GC/MS/MS) during the spring and summer of 2015 in surface water at 14 sampling sites in the mainstream of the Luanhe River to elucidate their seasonal distribution, composition, and potential sources. Results showed that total PAH concentrations in the surface water of the Luanhe River ranged from 33.33 ng·L-1 to 90.65 ng·L-1(52.64 ng·L-1 in average) in spring and 147.68 ng·L-1 to 252.68 ng·L-1 (169.88 ng·L-1 in average) in summer, respectively, and total concentrations of OCPs ranged from <0.08 ng·L-1 to 3.48 ng·L-1 (1.19 ng·L-1 in average) in spring and <0.08 to 5.47 ng·L-1(1.02 ng·L-1 in average) in summer, respectively. Seasonal pollution characteristics of PAHs in surface water during two different seasons showed that total PAH concentrations were much higher in summer than in spring at each sampling site on the Luanhe River. While seasonal pollution characteristics of OCPs showed that total OCP concentrations were much lower in spring than in summer at six sites including Luanxian, Daheiting reservoir dam, Panjiakou Village, Guojiatun, Qujiawan, and Baichengzi, and were higher in spring than in summer at the remaining eight sites. From the perspective of spatial and temporal variations in the composition patterns of PAHs and OCPs in surface water of the Luanhe River, the low and middle ring species of PAHs were dominant in spring and summer and the proportion of PAHs with different rings showed significant differences. Three-ring PAHs dominated the samples with 51.18% and 67.55% (61.39% on average) of total PAHs in spring, and four-ring and two-ring PAHs accounted for 11.78%-33.94% (20.97% on average) and 13.31%-27.12% (16.94% on average), respectively. In the summer, In the summer, naphthalene(Nap) was the main component of total PAHs at each sampling site and PAHs were predominated by two-ring compounds with 77.08% and 90.62% (83.34% on average) of the total, and by three-ring and four-ring compounds with 7.09%-15.22% (12.40% on average) and 2.23%-7.49% (3.97% on average), respectively. Only the residues of hexachlorocyclohexanes(HCHs) and dichlorodiphenyltrichloroethanes(DDTs) were detected in surface water of the Luanhe River at different degrees and HCHs were the dominant compounds. β-HCH was the main pollutant at most sampling sites with 43.78% and 70.09% (56.25% on average) of total HCHs in the spring and with 53.63% and 64.31% (58.37% on average) in the summer. α-HCH and γ-HCH were abundant at other sampling sites. Source analysis based on the isomer ratios indicated that PAHs in the Luanhe River mainly originated from combustion sources and also likely from petroleum processes. Ratios of OCPs confirmed that historical residues and long-range atmospheric transport were the major sources of HCHs in the study area, and new sources of lindane or γ-HCH existed at Wulongji and Sandaohezi in the spring and Daheting reservoir dam in the summer. Fresh inputs at the Panjiakou reservoir dam, Sandaohezi, Waigoumenzi, Baichengzi, Zhenglanqi, and the Shandianhe reservoir, and environmental residues at Jianggezhuang and Guojiatun were the major sources of DDTs. Concentrations of single PAHs in surface water of the Luanhe River did not exceed the water quality standards of China and other countries except that chrysene(Chr) exceeded the United States national water quality standard. Individual PAHs did not exceed any safety guidelines for aquatic organisms that are exposed to PAHs in water but total concentrations of PAHs exceeded the threshold limits set by the United States Environmental Protection Agency (EPA) and the European Union. This result indicated that consuming fish and other aquatic animals might pose a potential threat to human health due to the bioaccumulation of PAHs in aquatic organisms. The concentrations of OCPs in surface water of the Luanhe River did not exceed any water quality standards or the aquatic life threshold limits for freshwater developed by the EPA. However, the concentrations of α-HCH at Jianggezhuang, Wulongji, Qujiawan, and Baichengziand sites in the spring and at the Panjiakou reservoir dam, Panjiakou village, Qujiawan, and Baichengzi sites in the summer, and concentrations of p,p'-DDD at the Shandianhe reservoir and p,p'-DDE at Jianggezhuang, Sandaohezi, Guojiatun, and Shandianhe reservoir in the spring exceeded the human health ambient water quality criteria limit developed by the EPA. This result suggests that α-HCH, p,p'-DDE, and p,p'-DDD pose a potential health risk to the residents who live near the sampling sites on the Luanhe River. |
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