南方典型水源地及水产养殖区抗生素的复合污染特征及生态风险
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摘要
抗生素作为生长促进剂和疾病预防控制药物在水产养殖领域得到广泛应用,目前在许多环境水体中检测到不同类型的抗生素。环境中抗生素的残留问题也是目前环境研究的热点问题之一。本研究选择南方某市8个水源地和5个典型水产养殖区作为研究对象,采用固相萃取、高效液相色谱串联三重四级杆质谱联用仪方法,调查了32种常用抗生素在水体中的含量水平和空间分布特征,揭示了抗生素的来源,并对其生态风险进行了评价。水源地共检出12种抗生素,浓度范围为0.12～44.6 ng·L~(-1),以磺胺甲噁唑含量最高;水产养殖区检出14种抗生素,浓度范围为0.95～716 ng·L~(-1),以氯四环素检出浓度最高。整体上水产养殖区抗生素的浓度高于水源地。抗生素浓度与环境因子的冗余分析表明,水产养殖和生活污水排放是水体中抗生素的主要来源。对检出的13种抗生素进行生态风险评价,单一抗生素而言,环丙沙星、氧氟沙星、磺胺嘧啶、氯四环素和脱水红霉素的风险商值大于0.01而小于0.1,表现为低风险。总抗生素风险商值加和在大部分水源地大于0.01而小于0.1,表现为低风险;总抗生素风险商值加和在2个水产养殖区大于0.1,表现为中等风险,水产养殖区抗生素的长期生态风险应该引起关注。
Antibiotic pollution has attracted growing concerns, due to their extensive presence in the environment.Antibiotics are widely used in aquaculture to promote growth and prevent disease. The present study investigated the concentrations, spatial distributions, and sources of 32 commonly-used antibiotics in surface water from eightdrinking water sources and five typical aquaculture facilities in South China. The ecological risks of antibiotics in the study areas were also evaluated. Twelve antibiotics were detected in water samples from the water sources, with the concentrations ranging from 0.12 to 44.6 ng·L~(-1), and the highest concentrations were found for sulfamethoxazole. The concentrations of 14 antibiotics detected in aquaculture water ranged from 0.95 to 716 ng·L~(-1), and the highest concentrations were found for chlortetracycline. Overall, the concentrations of detected antibiotics at aquaculture sites were obviously higher than those in the water sources. Redundancy analysis between the antibiotic concentrations and environmental factors indicated that aquaculture and municipal sewage were the main source of antibiotics in the water. Risk assessment showed that for each single antibiotic detected in surface water, the risk quotients of ciprofloxacin, ofloxacin, sulfadiazine, chlortetracycline, and erythromycin-H2 O ranged from 0.01 to0.1,suggesting a low risk of these antibiotics. The total risk quotients also showed a low risk for most of the water sources(0.01-0.1). However, they were higher than 0.1 at two aquaculture sites indicating a medium risk.
Antibiotic pollution has attracted growing concerns, due to their extensive presence in the environment.Antibiotics are widely used in aquaculture to promote growth and prevent disease. The present study investigated the concentrations, spatial distributions, and sources of 32 commonly-used antibiotics in surface water from eightdrinking water sources and five typical aquaculture facilities in South China. The ecological risks of antibiotics in the study areas were also evaluated. Twelve antibiotics were detected in water samples from the water sources, with the concentrations ranging from 0.12 to 44.6 ng·L~(-1), and the highest concentrations were found for sulfamethoxazole. The concentrations of 14 antibiotics detected in aquaculture water ranged from 0.95 to 716 ng·L~(-1), and the highest concentrations were found for chlortetracycline. Overall, the concentrations of detected antibiotics at aquaculture sites were obviously higher than those in the water sources. Redundancy analysis between the antibiotic concentrations and environmental factors indicated that aquaculture and municipal sewage were the main source of antibiotics in the water. Risk assessment showed that for each single antibiotic detected in surface water, the risk quotients of ciprofloxacin, ofloxacin, sulfadiazine, chlortetracycline, and erythromycin-H2 O ranged from 0.01 to0.1,suggesting a low risk of these antibiotics. The total risk quotients also showed a low risk for most of the water sources(0.01-0.1). However, they were higher than 0.1 at two aquaculture sites indicating a medium risk.
引文
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[2] He L Y, Liu Y S, Su H C, et al. Dissemination of antibiotic resistance genes in representative broiler feedlots environments:Identification of indicator ARGs and correla-tions with environmental variables[J]. Environmental Science&Technology, 2014, 48(22):13120-13129
[3] Zhang Q Q, Ying G G, Pan C G, et al. Comprehensive evaluation of antibiotics emission and fate in the river basins of China:Source analysis, multimedia modeling, and linkage to bacterial resistance[J]. Environmental Science&Technology, 2015, 49(11):6772-6782
[4] Liu S, Ying G G, Zhang R Q, et al. Fate and occurrence of steroids in swine and dairy cattle farms with different farming scales and wastes disposal systems[J]. Environmental Pollution, 2012, 170:190-201
[5] Zhou L J, Ying G G, Zhao J L, et al. Trends in the occurrence of human and veterinary antibiotics in the sediments of the Yellow River, Hai River and Liao River in northern China[J]. Environmental Pollution, 2011, 159(7):1877-1885
[6] Liu X, Steele J C, Meng X Z. Usage, residue, and human health risk of antibiotics in Chinese aquaculture:A review[J]. Environmental Pollution, 2017, 223:161-169
[7] Zhou L J, Ying G G, Liu S, et al. Occurrence and fate of eleven classes of antibiotics in two typical wastewater treatment plants in South China[J]. Science of The Total Environment, 2013, 452-453:365-376
[8] Zhao S, Liu X, Cheng D, et al. Temporal-spatial variation and partitioning prediction of antibiotics in surface water and sediments from the intertidal zones of the Yellow River Delta, China[J]. Science of The Total Environment,2016, 569-570:1350-1358
[9] Yan C, Yang Y, Zhou J, et al. Antibiotics in the surface water of the Yangtze Estuary:Occurrence, distribution and risk assessment[J]. Environmental Pollution, 2013, 175:22-29
[10] Liang X, Chen B, Nie X, et al. The distribution and partitioning of common antibiotics in water and sediment of the Pearl River Estuary, South China[J]. Chemosphere,2013, 92(11):1410-1416
[11]朱婷婷,宋战锋,尹魁浩,等.深圳西丽水库抗生素残留现状及健康风险研究[J].环境污染与防治, 2014(5):49-53Zhu T T, Song Z F, Yin K H, et al. Study on current situation and health risk of antibiotics residue in source water of Xili Reservoir in Shenzhen[J]. Environmental Pollution and Control, 2014(5):49-53(in Chinese)
[12]李兆新,董晓,吴蒙蒙,等.黄海桑沟湾养殖区海水中喹诺酮类抗生素的残留状况[J].海洋环境科学, 2018(2):182-186Li Z X, Dong X, Wu M M, et al. Quinolone residues in seawater of aquaculture area, Sanggou Bay, Yellow Sea,China[J]. Marine Environmental Science, 2018(2):182-186(in Chinese)
[13]金磊,姜蕾,韩琪,等.华东地区某水源水中13种磺胺类抗生素的分布特征及人体健康风险评价[J].环境科学, 2016(7):2515-2521Jin L, Jiang L, Han Q, et al. Distribution characteristics and health risk assessment of thirteen sulfonamides antibiotics in a drinking water source in East China[J]. Environmental Science, 2016(7):2515-2521(in Chinese)
[14]梁惜梅,施震,黄小平.珠江口典型水产养殖区抗生素的污染特征[J].生态环境学报, 2013(2):304-310Liang X M, Shi Z, Huang X P, et al. Occurrence of antibiotics in typical aquaculture of the Pearl River Estuary[J].Ecology and Environment Sciences, 2013(2):304-310(in Chinese)
[15]李经纬,丁紫荣,余乐洹,等.高效液相色谱-串联质谱法同时检测水中抗生素[J].分析科学学报, 2016(6):851-856Li J W, Ding Z R, Yu L H, et al. Determination of seventeen antibiotics in water by liquid chromatography-tandem mass spectrometry[J]. Journal of Analytical Science,2016(6):851-856(in Chinese)
[16]周志洪,赵建亮,魏晓东,等.珠江广州段水体抗生素的复合污染特征及其生态风险[J].生态环境学报,2017(6):1034-1041Zhou Z H, Zhao J L, Wei X D, et al. Co-occurrence and ecological risk of antibiotics in surface water of Guangzhou Section of Pearl River[J]. Ecology and Environment Sciences, 2017(6):1034-1041(in Chinese)
[17] Wang Z, Du Y, Yang C, et al. Occurrence and ecological hazard assessment of selected antibiotics in the surface waters in and around Lake Honghu, China[J]. Science of The Total Environment, 2017, 609:1423-1432
[18] Ma Y, Li M, Wu M, et al. Occurrences and regional distributions of 20 antibiotics in water bodies during groundwater recharge[J]. Science of The Total Environment,2015, 518-519:498-506
[19] Lin A Y-C, Yu T-H, Lin C-F. Pharmaceutical contamination in residential, industrial, and agricultural waste streams:Risk to aqueous environments in Taiwan[J].Chemosphere, 2008, 74(1):131-141
[20] Liu W R, Zhao J L, Liu Y S, et al. Biocides in the Yangtze River of China:Spatiotemporal distribution, mass load and risk assessment[J]. Environmental Pollution,2015, 200:53-63
[21]赵建亮,应光国,魏东斌,等.水体和沉积物中毒害污染物的生态风险评价方法体系研究进展[J].生态毒理学报, 2011, 6(6):577-588Zhao J L, Ying G G, Wei D B, et al. Ecological risk assessment methodology of toxic pollutants in surface water and sediments:A review[J]. Asian Journal of Ecotoxicology, 2011, 6(6):577-588(in Chinese)
[22] Hernando M D, Mezcua M, Fernández-Alba A R, et al.Environmental risk assessment of pharmaceutical residues in wastewater effluents, surface waters and sediments[J].Talanta, 2006, 69(2):334-342
[23]武旭跃,邹华,朱荣,等.太湖贡湖湾水域抗生素污染特征分析与生态风险评价[J].环境科学, 2016(12):4596-4604Wu X Y, Zou H, Zhu R, et al. Occurrence, distribution and ecological risk of antibiotics in surface water of the Gonghu Bay, Taihu Lake[J]. Environmental Science,2016(12):4596-4604(in Chinese)
[24]胡冠九,穆肃,赵永刚,等.南京典型县区饮用水源抗生素含量特征[J].环境化学, 2015(1):192-193
[25] Zhang R, Zhang G, Zheng Q, et al. Occurrence and risks of antibiotics in the Laizhou Bay, China:Impacts of river discharge[J]. Ecotoxicology and Environmental Safety,2012, 80:208-215
[26] Zou S, Xu W, Zhang R, et al. Occurrence and distribution of antibiotics in coastal water of the Bohai Bay, China:Impacts of river discharge and aquaculture activities[J].Environmental Pollution, 2011, 159(10):2913-2920
[27]郝勤伟,徐向荣,陈辉,等.广州市南沙水产养殖区抗生素的残留特性[J].热带海洋学报, 2017(1):106-113Hao Q W, Xu X R, Chen H, et al. Residual antibiotics in the Nansha aquaculture area of Guangzhou[J]. Journal of Tropical Oceanography, 2017(1):106-113(in Chinese)
[28]王瑞旋,陈毕生.喹诺酮类药物在水产养殖中的应用研究概况[J].南方水产, 2007(3):73-79Wang R X, Chen B S. Review on applied research of quinolones in aquaculture[J]. South China Fisheries Science, 2007(3):73-79(in Chinese)
[29]赵永宏,邓祥征,吴锋,等.乌梁素海流域氮磷减排与区域经济发展的均衡分析[J].环境科学研究, 2011(1):110-117Zhao Y H, Deng X Z, Wu F, et al. Equilibrium analysis between nitrogen and phosphorus emission reduction and regional economic development of Wuliangsuhai Watershed[J]. Research of Environmental Sciences, 2011(1):110-117(in Chinese)
[2] He L Y, Liu Y S, Su H C, et al. Dissemination of antibiotic resistance genes in representative broiler feedlots environments:Identification of indicator ARGs and correla-tions with environmental variables[J]. Environmental Science&Technology, 2014, 48(22):13120-13129
[3] Zhang Q Q, Ying G G, Pan C G, et al. Comprehensive evaluation of antibiotics emission and fate in the river basins of China:Source analysis, multimedia modeling, and linkage to bacterial resistance[J]. Environmental Science&Technology, 2015, 49(11):6772-6782
[4] Liu S, Ying G G, Zhang R Q, et al. Fate and occurrence of steroids in swine and dairy cattle farms with different farming scales and wastes disposal systems[J]. Environmental Pollution, 2012, 170:190-201
[5] Zhou L J, Ying G G, Zhao J L, et al. Trends in the occurrence of human and veterinary antibiotics in the sediments of the Yellow River, Hai River and Liao River in northern China[J]. Environmental Pollution, 2011, 159(7):1877-1885
[6] Liu X, Steele J C, Meng X Z. Usage, residue, and human health risk of antibiotics in Chinese aquaculture:A review[J]. Environmental Pollution, 2017, 223:161-169
[7] Zhou L J, Ying G G, Liu S, et al. Occurrence and fate of eleven classes of antibiotics in two typical wastewater treatment plants in South China[J]. Science of The Total Environment, 2013, 452-453:365-376
[8] Zhao S, Liu X, Cheng D, et al. Temporal-spatial variation and partitioning prediction of antibiotics in surface water and sediments from the intertidal zones of the Yellow River Delta, China[J]. Science of The Total Environment,2016, 569-570:1350-1358
[9] Yan C, Yang Y, Zhou J, et al. Antibiotics in the surface water of the Yangtze Estuary:Occurrence, distribution and risk assessment[J]. Environmental Pollution, 2013, 175:22-29
[10] Liang X, Chen B, Nie X, et al. The distribution and partitioning of common antibiotics in water and sediment of the Pearl River Estuary, South China[J]. Chemosphere,2013, 92(11):1410-1416
[11]朱婷婷,宋战锋,尹魁浩,等.深圳西丽水库抗生素残留现状及健康风险研究[J].环境污染与防治, 2014(5):49-53Zhu T T, Song Z F, Yin K H, et al. Study on current situation and health risk of antibiotics residue in source water of Xili Reservoir in Shenzhen[J]. Environmental Pollution and Control, 2014(5):49-53(in Chinese)
[12]李兆新,董晓,吴蒙蒙,等.黄海桑沟湾养殖区海水中喹诺酮类抗生素的残留状况[J].海洋环境科学, 2018(2):182-186Li Z X, Dong X, Wu M M, et al. Quinolone residues in seawater of aquaculture area, Sanggou Bay, Yellow Sea,China[J]. Marine Environmental Science, 2018(2):182-186(in Chinese)
[13]金磊,姜蕾,韩琪,等.华东地区某水源水中13种磺胺类抗生素的分布特征及人体健康风险评价[J].环境科学, 2016(7):2515-2521Jin L, Jiang L, Han Q, et al. Distribution characteristics and health risk assessment of thirteen sulfonamides antibiotics in a drinking water source in East China[J]. Environmental Science, 2016(7):2515-2521(in Chinese)
[14]梁惜梅,施震,黄小平.珠江口典型水产养殖区抗生素的污染特征[J].生态环境学报, 2013(2):304-310Liang X M, Shi Z, Huang X P, et al. Occurrence of antibiotics in typical aquaculture of the Pearl River Estuary[J].Ecology and Environment Sciences, 2013(2):304-310(in Chinese)
[15]李经纬,丁紫荣,余乐洹,等.高效液相色谱-串联质谱法同时检测水中抗生素[J].分析科学学报, 2016(6):851-856Li J W, Ding Z R, Yu L H, et al. Determination of seventeen antibiotics in water by liquid chromatography-tandem mass spectrometry[J]. Journal of Analytical Science,2016(6):851-856(in Chinese)
[16]周志洪,赵建亮,魏晓东,等.珠江广州段水体抗生素的复合污染特征及其生态风险[J].生态环境学报,2017(6):1034-1041Zhou Z H, Zhao J L, Wei X D, et al. Co-occurrence and ecological risk of antibiotics in surface water of Guangzhou Section of Pearl River[J]. Ecology and Environment Sciences, 2017(6):1034-1041(in Chinese)
[17] Wang Z, Du Y, Yang C, et al. Occurrence and ecological hazard assessment of selected antibiotics in the surface waters in and around Lake Honghu, China[J]. Science of The Total Environment, 2017, 609:1423-1432
[18] Ma Y, Li M, Wu M, et al. Occurrences and regional distributions of 20 antibiotics in water bodies during groundwater recharge[J]. Science of The Total Environment,2015, 518-519:498-506
[19] Lin A Y-C, Yu T-H, Lin C-F. Pharmaceutical contamination in residential, industrial, and agricultural waste streams:Risk to aqueous environments in Taiwan[J].Chemosphere, 2008, 74(1):131-141
[20] Liu W R, Zhao J L, Liu Y S, et al. Biocides in the Yangtze River of China:Spatiotemporal distribution, mass load and risk assessment[J]. Environmental Pollution,2015, 200:53-63
[21]赵建亮,应光国,魏东斌,等.水体和沉积物中毒害污染物的生态风险评价方法体系研究进展[J].生态毒理学报, 2011, 6(6):577-588Zhao J L, Ying G G, Wei D B, et al. Ecological risk assessment methodology of toxic pollutants in surface water and sediments:A review[J]. Asian Journal of Ecotoxicology, 2011, 6(6):577-588(in Chinese)
[22] Hernando M D, Mezcua M, Fernández-Alba A R, et al.Environmental risk assessment of pharmaceutical residues in wastewater effluents, surface waters and sediments[J].Talanta, 2006, 69(2):334-342
[23]武旭跃,邹华,朱荣,等.太湖贡湖湾水域抗生素污染特征分析与生态风险评价[J].环境科学, 2016(12):4596-4604Wu X Y, Zou H, Zhu R, et al. Occurrence, distribution and ecological risk of antibiotics in surface water of the Gonghu Bay, Taihu Lake[J]. Environmental Science,2016(12):4596-4604(in Chinese)
[24]胡冠九,穆肃,赵永刚,等.南京典型县区饮用水源抗生素含量特征[J].环境化学, 2015(1):192-193
[25] Zhang R, Zhang G, Zheng Q, et al. Occurrence and risks of antibiotics in the Laizhou Bay, China:Impacts of river discharge[J]. Ecotoxicology and Environmental Safety,2012, 80:208-215
[26] Zou S, Xu W, Zhang R, et al. Occurrence and distribution of antibiotics in coastal water of the Bohai Bay, China:Impacts of river discharge and aquaculture activities[J].Environmental Pollution, 2011, 159(10):2913-2920
[27]郝勤伟,徐向荣,陈辉,等.广州市南沙水产养殖区抗生素的残留特性[J].热带海洋学报, 2017(1):106-113Hao Q W, Xu X R, Chen H, et al. Residual antibiotics in the Nansha aquaculture area of Guangzhou[J]. Journal of Tropical Oceanography, 2017(1):106-113(in Chinese)
[28]王瑞旋,陈毕生.喹诺酮类药物在水产养殖中的应用研究概况[J].南方水产, 2007(3):73-79Wang R X, Chen B S. Review on applied research of quinolones in aquaculture[J]. South China Fisheries Science, 2007(3):73-79(in Chinese)
[29]赵永宏,邓祥征,吴锋,等.乌梁素海流域氮磷减排与区域经济发展的均衡分析[J].环境科学研究, 2011(1):110-117Zhao Y H, Deng X Z, Wu F, et al. Equilibrium analysis between nitrogen and phosphorus emission reduction and regional economic development of Wuliangsuhai Watershed[J]. Research of Environmental Sciences, 2011(1):110-117(in Chinese)