截污调水后滇池表层沉积物中16种PAHs的分布特征
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摘要
截污调水等工程实施后,滇池的外源污染已得到有效控制,表层沉积物等内源污染物应加以重视.为研究滇池表层沉积物中16种多环芳烃(PAHs)的分布特征,采用气相色谱-质谱联用法(GC-MS)分析了2016年12月采集的19个滇池表层沉积物样品的PAHs含量,解析其时空分布规律、来源及生态风险.滇池表层沉积物中总多环芳烃(TPAHs)的含量范围为92. 31～1 546. 78 ng·g~(-1),平均值为496. 30 ng·g~(-1),草海TPAHs含量(平均932. 37 ng·g~(-1))远高于外海(平均380. 02ng·g~(-1)),随着截污调水工程的开展,TPAHs含量较2012年大幅下降,已处于我国重点水域中较低水平.滇池表层沉积物中含量最高的物质为荧蒽(80. 65 ng·g~(-1)),毒性当量(TEQ)含量最高的物质为二苯并[a,h]蒽(42. 97 ng·g~(-1)). PAHs组成以4环及5～6环为主(分别占总含量的40. 38%和40. 22%),PAHs构成较以往大体一致.分子比值法分析结果表明,滇池表层沉积物中PAHs主要由生物质或煤的燃烧贡献.基于潜在生态风险标志对比法评估,全湖总体处于低风险水平,但草海的生态风险相对较高,值得进一步关注.本研究结果可为滇池水质的保持与提升提供基础数据和重要参考.
The external pollution of Dianchi Lake has been effectively controlled with the implementation of the integrated water environment control project. However,further attention should be paid to endogenous pollutants,such as surface sediments. To investigate the distribution of 16 polycyclic aromatic hydrocarbons( PAHs) in surface sediments of Dianchi Lake,PAH concentrations in 19 surface sediment samples( collected in December 2016) were quantitatively measured by gas chromatography-mass spectrometry( GC-MS). The spatial and temporal distribution,sources,and ecological risks were also analyzed. The concentration of total PAHs( TPAHs) in the Dianchi Lake surface sediments varied in the range of 92. 31-1546. 78 ng·g~(-1) with an average of 496. 30 ng·g~(-1). The average concentration of TPAHs in the surface sediments from Caohai( 932. 37 ng·g~(-1)) was much greater than that from Waihai( 380. 02 ng·g~(-1)). With the implement of the integrated water environment control project,the concentration of TPAHs in the surface sediments from Dianchi Lake was significantly lower than those detected in 2012,and was already relatively low level among other key waterbodies in China. The PAH with the highest concentration was fluoranthene( 80. 65 ng·g~(-1)) and the substance with the highest toxic equivalent quantity( TEQ) was dibenz[a,h] anthracene( 42. 97 ng·g~(-1)). The PAHs were mainly composed of 4 ring and 5-6 ring compounds( with the concentration ratio of 40. 38% and 40. 22%,respectively),which indicated that the proportions of middlering and high-ring compounds were generally consistent. The results of the molecular diagnostic ratio analysis showed that the primary source of PAHs in Dianchi Lake surface sediments are biomass and coal combustion. Based on the potential ecological risk marker comparison method,the entire lake was classified as having a low ecological risk,while the ecological risk of Caohai was relatively higher,which should be concerned further. The results provide initial data and act as an important reference for the conservation and improvement of water quality in Dianchi Lake.
The external pollution of Dianchi Lake has been effectively controlled with the implementation of the integrated water environment control project. However,further attention should be paid to endogenous pollutants,such as surface sediments. To investigate the distribution of 16 polycyclic aromatic hydrocarbons( PAHs) in surface sediments of Dianchi Lake,PAH concentrations in 19 surface sediment samples( collected in December 2016) were quantitatively measured by gas chromatography-mass spectrometry( GC-MS). The spatial and temporal distribution,sources,and ecological risks were also analyzed. The concentration of total PAHs( TPAHs) in the Dianchi Lake surface sediments varied in the range of 92. 31-1546. 78 ng·g~(-1) with an average of 496. 30 ng·g~(-1). The average concentration of TPAHs in the surface sediments from Caohai( 932. 37 ng·g~(-1)) was much greater than that from Waihai( 380. 02 ng·g~(-1)). With the implement of the integrated water environment control project,the concentration of TPAHs in the surface sediments from Dianchi Lake was significantly lower than those detected in 2012,and was already relatively low level among other key waterbodies in China. The PAH with the highest concentration was fluoranthene( 80. 65 ng·g~(-1)) and the substance with the highest toxic equivalent quantity( TEQ) was dibenz[a,h] anthracene( 42. 97 ng·g~(-1)). The PAHs were mainly composed of 4 ring and 5-6 ring compounds( with the concentration ratio of 40. 38% and 40. 22%,respectively),which indicated that the proportions of middlering and high-ring compounds were generally consistent. The results of the molecular diagnostic ratio analysis showed that the primary source of PAHs in Dianchi Lake surface sediments are biomass and coal combustion. Based on the potential ecological risk marker comparison method,the entire lake was classified as having a low ecological risk,while the ecological risk of Caohai was relatively higher,which should be concerned further. The results provide initial data and act as an important reference for the conservation and improvement of water quality in Dianchi Lake.
引文
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[25]高秋生,焦立新,杨柳,等.白洋淀典型持久性有机污染物污染特征与风险评估[J].环境科学,2018,39(4):1616-1627.Gao Q S,Jiao L X,Yang L,et al.Occurrence and ecological risk assessment of typical persistent organic pollutants in Baiyangdian Lake[J].Environmental Science,2018,39(4):1616-1627.
[26]王乙震,张世禄,孔凡青,等.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[J].环境科学,2017,38(10):4194-4211.Wang Y Z,Zhang S L,Kong F Q,et al.Seasonal distribution,composition,and source apportionment of polycyclic aromatic hydrocarbons and organochlorine pesticides in the main stream of the Luanhe River[J].Environmental Science,2017,38(10):4194-4211.
[27]Zeng E Y,Vista C L.Organic pollutants in the coastal environment off San Diego,California.1.Source identification and assessment by compositional indices of polycyclic aromatic hydrocarbons[J].Environmental Toxicology and Chemistry,1997,16(2):179-188.
[28]Mai B X,Fu J M,Sheng G Y,et al.Chlorinated and polycyclic aromatic hydrocarbons in riverine and estuarine sediments from Pearl River Delta,China[J].Environmental Pollution,2002,117(3):457-474.
[29]Yunker M B,Macdonald R W,Goyette D,et al.Natural and anthropogenic inputs of hydrocarbons to the Strait of Georgia[J].Science of the Total Environment,1999,225(3):181-209.
[30]Yunker M B,Macdonald R W,Vingarzan R,et al.PAHs in the Fraser River basin:a critical appraisal of PAH ratios as indicators of PAH source and composition[J].Organic Geochemistry,2002,33(4):489-515.
[31]Long E R,Macdonald D D,Smith S L,et al.Incidence of adverse biological effects within ranges of chemical concentrations in marine and estuarine sediments[J].Environmental Management,1995,19(1):81-97.
[2]Readman J W,Fillmann G,Tolosa I,et al.Petroleum and PAHcontamination of the Black Sea[J].Marine Pollution Bulletin,2002,44(1):48-62.
[3]Kang M J,Yang F,Ren H,et al.Influence of continental organic aerosols to the marine atmosphere over the East China Sea:insights from lipids,PAHs and phthalates[J].Science of the Total Environment,2017,607-608:339-350.
[4]Zhang Y X,Tao S,Shen H Z,et al.Inhalation exposure to ambient polycyclic aromatic hydrocarbons and lung cancer risk of Chinese population[J].Proceedings of the National Academy of Sciences of the United States of America,2009,106(50):21063-21067.
[5]Wang Z C,Liu M,Yang Y.Characterization and sources analysis of polycyclic aromatic hydrocarbons in surface sediments in the Yangtze River Estuary[J].Environmental Earth Sciences,2015,73(5):2453-2462.
[6]Wang M,Wang C Y,Li Y W.Petroleum hydrocarbons in a water-sediment system from Yellow River estuary and adjacent coastal area,China:distribution pattern,risk assessment and sources[J].Marine Pollution Bulletin,2017,122(1-2):139-148.
[7]Zhao Z H,Zhang L,Wu J L.Polycyclic aromatic hydrocarbons(PAHs)and organochlorine pesticides(OCPs)in sediments from lakes along the middle-lower reaches of the Yangtze River and the Huaihe River of China[J].Limnology and Oceanography,2016,61(1):47-60.
[8]He Y,Meng W,Xu J,et al.Spatial distribution and potential toxicity of polycyclic aromatic hydrocarbons in sediments from Liaohe River Basin,China[J].Environmental Monitoring and Assessment,2016,188(3):193.
[9]Qian X,Liang B C,Liu X,et al.Distribution,sources,and ecological risk assessment of polycyclic aromatic hydrocarbons in surface sediments from the Haihe River,a typical polluted urban river in Northern China[J].Environmental Science and Pollution Research,2017,24(20):17153-17165.
[10]Zhao Z H,Jiang Y,Li Q Y,et al.Spatial correlation analysis of polycyclic aromatic hydrocarbons(PAHs)and organochlorine pesticides(OCPs)in sediments between Taihu Lake and its tributary rivers[J].Ecotoxicology and Environmental Safety,2017,142:117-128.
[11]Liu C,Zhang L,Fan C X,et al.Temporal occurrence and sources of persistent organic pollutants in suspended particulate matter from the most heavily polluted river mouth of Lake Chaohu,China[J].Chemosphere,2017,174:39-45.
[12]Weng J,Li S,Wang T C,et al.Distribution of petroleum hydrocarbons in sediments from Dianchi Lake,China[J].Environmental Earth Sciences,2016,75(6):456.
[13]Zhao S M,Wang B,Wang D W,et al.Environmental behavior of PAHs in Dianchi Lake distributions,sources and risk assessment of polycyclic aromatic hydrocarbons in surface sediments from Dianchi Lake,China[J].International Journal of Environmental Research,2014,8(2):317-328.
[14]Guo J Y,Wu F C,Liao H Q,et al.Sedimentary record of polycyclic aromatic hydrocarbons and DDTs in Dianchi Lake,an urban lake in Southwest China[J].Environmental Science and Pollution Research,2013,20(8):5471-5480.
[15]Ma X H,Han X X,Jiang Q L,et al.Historical records and source apportionment of polycyclic aromatic hydrocarbons over the past 100 years in Dianchi Lake,a plateau lake in Southwest China[J].Archives of Environmental Contamination and Toxicology,2018,75(2):187-198.
[16]Sun P P,Xie B,Song Y M,et al.Historical trends of polycyclic aromatic hydrocarbons in the reservoir sediment of the Dianchi Watershed,Southwest China[J].Bulletin of Environmental Contamination and Toxicology,2017,99(1):117-124.
[17]Dai C,Tan Q,Lu W T,et al.Identification of optimal water transfer schemes for restoration of a eutrophic lake:an integrated simulation-optimization method[J].Ecological Engineering,2016,95:409-421.
[18]董磊,汤显强,林莉,等.长江武汉段丰水期水体和沉积物中多环芳烃及邻苯二甲酸酯类有机污染物污染特征及来源分析[J].环境科学,2018,39(6):2588-2599.Dong L,Tang X Q,Lin L,et al.Pollution characteristics and source identification of polycyclic aromatic hydrocarbons and phthalic acid esters during high water level periods in the Wuhan Section of the Yangtze River,China[J].Environmental Science,2018,39(6):2588-2599.
[19]刘少鹏,李先国,张大海,等.墨水河表层沉积物中多环芳烃(PAHs)的分布特征、来源解析及生态风险评价[J].环境化学,2018,37(4):843-850.Liu S P,Li X G,Zhang D H,et al.Distribution,source and ecological risk assessment of polycyclic aromatic hydrocarbons(PAHs)in surface sediments from Moshui River[J].Environmental Chemistry,2018,37(4):843-850.
[20]Li Q,Xu X,Fang Y Y,et al.The temporal changes of the concentration level of typical toxic organics in the river sediments around Beijing[J].Frontiers of Environmental Science&Engineering,2018,12(6):8.
[21]Yang J,Yang Y,Chen R S,et al.Modeling and evaluating spatial variation of polycyclic aromatic hydrocarbons in urban lake surface sediments in Shanghai[J].Environmental Pollution,2018,235:1-10.
[22]吴义国,方冰芯,李玉成,等.杭埠-丰乐河表层沉积物中多环芳烃的污染特征、来源分析及生态风险评价[J].环境化学,2017,36(2):420-429.Wu Y G,Fang B X,Li Y C,et al.Occurrence of polycyclic aromatic hydrocarbons(PAHs)in surface sediments from Hangbu-Fengle River:pollution characteristics,potential source and risk assessment[J].Environmental Chemistry,2017,36(2):420-429.
[23]江敏,Tuan L H,梅卫平,等.舟山近海水体和沉积物中多环芳烃分布特征[J].环境科学,2014,35(7):2672-2679.Jiang M,Tuan L H,Mei W P,et al.Distribution of polycyclic aromatic hydrocarbons in water and sediment from Zhoushan Coastal Area,China[J].Environmental Science,2014,35(7):2672-2679.
[24]张家泉,胡天鹏,邢新丽,等.大冶湖表层沉积物-水中多环芳烃的分布、来源及风险评价[J].环境科学,2017,38(1):170-179.Zhang J Q,Hu T P,Xing X L,et al.Distribution,sources and risk assessment of the PAHs in the surface sediments and water from the Daye Lake[J].Environmental Science,2017,38(1):170-179.
[25]高秋生,焦立新,杨柳,等.白洋淀典型持久性有机污染物污染特征与风险评估[J].环境科学,2018,39(4):1616-1627.Gao Q S,Jiao L X,Yang L,et al.Occurrence and ecological risk assessment of typical persistent organic pollutants in Baiyangdian Lake[J].Environmental Science,2018,39(4):1616-1627.
[26]王乙震,张世禄,孔凡青,等.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[J].环境科学,2017,38(10):4194-4211.Wang Y Z,Zhang S L,Kong F Q,et al.Seasonal distribution,composition,and source apportionment of polycyclic aromatic hydrocarbons and organochlorine pesticides in the main stream of the Luanhe River[J].Environmental Science,2017,38(10):4194-4211.
[27]Zeng E Y,Vista C L.Organic pollutants in the coastal environment off San Diego,California.1.Source identification and assessment by compositional indices of polycyclic aromatic hydrocarbons[J].Environmental Toxicology and Chemistry,1997,16(2):179-188.
[28]Mai B X,Fu J M,Sheng G Y,et al.Chlorinated and polycyclic aromatic hydrocarbons in riverine and estuarine sediments from Pearl River Delta,China[J].Environmental Pollution,2002,117(3):457-474.
[29]Yunker M B,Macdonald R W,Goyette D,et al.Natural and anthropogenic inputs of hydrocarbons to the Strait of Georgia[J].Science of the Total Environment,1999,225(3):181-209.
[30]Yunker M B,Macdonald R W,Vingarzan R,et al.PAHs in the Fraser River basin:a critical appraisal of PAH ratios as indicators of PAH source and composition[J].Organic Geochemistry,2002,33(4):489-515.
[31]Long E R,Macdonald D D,Smith S L,et al.Incidence of adverse biological effects within ranges of chemical concentrations in marine and estuarine sediments[J].Environmental Management,1995,19(1):81-97.