天津供水系统中抗生素分布变化特征与健康风险评价
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摘要
通过采用固相萃取富集法和液相色谱质谱联用技术对天津市供水系统中净水厂和管网中的6类10种抗生素浓度水平进行了分析,研究了抗生素在各处理工艺单元后的变化特征,以及在管网中的分布迁移规律,并进行了健康风险评价.对不同处理工艺的A、B两水厂中抗生素的检测结果显示:采用传统处理工艺的A水厂出水中抗生素的质量浓度范围为0.96~126.43 ng·L~(-1),总去除率为-46.47%~45.10%,混凝工艺对抗生素物质的去除起主要作用;具有深度处理工艺的B水厂出水中抗生素的浓度为ND~72.27 ng·L~(-1),其中罗红霉素未检出,抗生素的去除效率为40.25%~70.33%,明显优于A水厂,紫外+氯消毒工艺对抗生素的去除最为明显.给水管网中抗生素浓度分析结果表明:10种抗生素中除罗红霉素检出率为75.0%外,其余均为100.0%.抗生素浓度范围为ND~348.99 ng·L~(-1),浓度随管段的延伸而逐渐降低,其衰减符合一级反应动力学模型.基于蒙特卡洛法对饮用水中抗生素的致癌风险和非致癌风险进行了评估,结果表明均处于可接受风险水平.
Six groups of 10 antibiotics in the water plants and water supply network in Tianjin were sampled and analyzed by using solid phase extraction and high performance liquid chromatography-mass spectrometry.The concentrations of 10 antibiotics were detected in the water treatment process units,and the distribution,migration,and health risk assessment in the water supply networks were studied.The results of antibiotic determination in the water plants showed that the antibiotic concentrations were 0.96-126.43 ng·L~(-1),and the removal efficiency was-46.47%-45.10% in plant A using traditional treatment processes.The coagulation treatment process was effective for the antibiotic removal in plant A.In plant B with an advanced treatment process,roxithromycin was not detected,and the concentration of other antibiotics was ND-72.27 ng·L~(-1).The removal efficiency of the antibiotics was 40.25%-70.33% in plant B,which was remarkably higher than that in plant A.The results indicated the process of UV combined with chlorine disinfection played a major role in removing antibiotics in plant B.In addition,the antibiotic distribution in the water pipes indicated that the detection rate of roxithromycin was 75.0% and that for other antibiotics was 100.0%.The concentration of 10 antibiotics was ND-348.99 ng·L~(-1) and decreased gradually with the increase of the transmission distance,which followed the first order reaction kinetics model.Based on the Monte Carlo method,the carcinogenic and non-carcinogenic health risks of antibiotics in drinking water were assessed.The results displayed that both were at an acceptable level of risk.
Six groups of 10 antibiotics in the water plants and water supply network in Tianjin were sampled and analyzed by using solid phase extraction and high performance liquid chromatography-mass spectrometry.The concentrations of 10 antibiotics were detected in the water treatment process units,and the distribution,migration,and health risk assessment in the water supply networks were studied.The results of antibiotic determination in the water plants showed that the antibiotic concentrations were 0.96-126.43 ng·L~(-1),and the removal efficiency was-46.47%-45.10% in plant A using traditional treatment processes.The coagulation treatment process was effective for the antibiotic removal in plant A.In plant B with an advanced treatment process,roxithromycin was not detected,and the concentration of other antibiotics was ND-72.27 ng·L~(-1).The removal efficiency of the antibiotics was 40.25%-70.33% in plant B,which was remarkably higher than that in plant A.The results indicated the process of UV combined with chlorine disinfection played a major role in removing antibiotics in plant B.In addition,the antibiotic distribution in the water pipes indicated that the detection rate of roxithromycin was 75.0% and that for other antibiotics was 100.0%.The concentration of 10 antibiotics was ND-348.99 ng·L~(-1) and decreased gradually with the increase of the transmission distance,which followed the first order reaction kinetics model.Based on the Monte Carlo method,the carcinogenic and non-carcinogenic health risks of antibiotics in drinking water were assessed.The results displayed that both were at an acceptable level of risk.
引文
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[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,2016,37(7):2515-2521.Jin 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,2016,37(7):2515-2521.
[14]姜蕾,崔长征,黄岭.典型抗生素在饮用水厂的去除特征与健康风险[J].净水技术,2016,35(S1):100-103,121.)Jiang L,Cui C Z,Huang L.Removal of antibiotics in drinking water processes and their health risk[J].Water Purification Technology,2016,35(S1):100-103,121.
[15]Zhang X B,Guo W S,Ngo H H,et al.Performance evaluation of powdered activated carbon for removing 28 types of antibiotics from water[J].Journal of Environmental Management,2016,172:193-200.
[16]吴熊勋.城市水环境污染控制[M].南京:东南大学出版社,1989.
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[18]张应华,刘志全,李广贺,等.基于不确定性分析的健康环境风险评价[J].环境科学,2007,28(7):1409-1415.Zhang Y H,Liu Z Q,Li G H,et al.Uncertainty analysis of health risk assessment caused by benzene contamination in a contaminated site[J].Environmental Science,2007,28(7):1409-1415.
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[20]Zeise L,Wilson R,Crouch E.Use of acute toxicity to estimate carcinogenic risk[J].Risk Analysis,1984,4(3):187-199.
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[22]Strenge D,Chamberlain P J.Multimedia environmental pollutant assessment system(MEPAs):exposure pathway and human health impact assessment models[M].Richland,WA:Pacific Northwest Laboratory,1995.
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[24]Layton D,Mallon B,Rosenblatt D,et al.Deriving allowable daily intakes for systemic toxicants lacking chronic toxicity data[J].Regulatory Toxicology and Pharmacology,1987,7(1):96-112.
[25]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.
[26]Dean R G.Compatibility of borrow material for beach fills[C].Coastal Engineering(1974).ASCE,2012.1319-1333.
[27]Zuccato E,Bagnati R,Fioretti F,et al.Environmental loads and detection of pharmaceuticals in Italy[A].In:Kümmerer K(Ed.).Pharmaceuticals in the Environment[M].Berlin Heidelberg:Springer,2001.19-27.
[28]崔亚丰,何江涛,苏思慧,等.某市典型地段地表水及地下水中氟喹诺酮类抗生素分布特征[J].环境科学,2015,36(11):4060-4067.Cui Y F,He J T,Su S H,et al.Distribution characteristics of fluoroquinolones antibiotics in surface water and groundwater from typical areas in a city[J].Environmental Science,2015,36(11):4060-4067.
[29]王冉,刘铁铮,王恬.抗生素在环境中的转归及其生态毒性[J].生态学报,2006,26(1):265-270.Wang R,Liu T Z,Wang T.The fate of antibiotics in environment and its ecotoxicology:a review[J].Acta Ecologica Sinica,2006,26(1):265-270.
[30]Qiao T J,Yu Z R,Zhang X H,et al.Occurrence and fate of pharmaceuticals and personal care products in drinking water in southern China[J].Journal of Environmental Monitoring,2011,13(11):3097-3103.
[31]Straub J O.Aquatic environmental risk assessment for human use of the old antibiotic sulfamethoxazole in Europe[J].Environmental Toxicology and Chemistry,2015,35(4):767-779.
[32]Dodd M C,Huang C H.Transformation of the antibacterial agent sulfamethoxazole in reactions with chlorine:kinetics,mechanisms,and pathways[J].Environmental Science&Technology,2004,38(21):5607-5615.
[33]Vieno N M,Hrkki H,Tuhkanen T,et al.Occurrence of pharmaceuticals in river water and their elimination in a pilotscale drinking water treatment plant[J].Environmental Science&Technology,2007,41(14):5077-5084.
[34]Li K X,Yediler A,Yang M,et al.Ozonation of oxytetracycline and toxicological assessment of its oxidation by-products[J].Chemosphere,2008,72(3):473-478.
[35]Turiel E,Bordin G,Rodríguez A R.Study of the evolution and degradation products of ciprofloxacin and oxolinic acid in river water samples by HPLC-UV/MS/MS-MS[J].Journal of Environmental Monitoring,2005,7(3):189-195.
[36]李耀中,孔欣,周岳溪,等.光催化降解三类难降解有机工业废水[J].中国给水排水,2003,19(1):5-8.Li Y Z,Kong X,Zhou Y X,et al.Photocatalytic degradation of three kinds of refractory industrial organic wastewater[J].China Water&Wastewater,2003,19(1):5-8.
[37]宋晨怡,尹大强.四环素光催化降解特性与选择性研究[J].环境科学,2014,35(2):619-625.Song C Y,Yin D Q.Characteristics and selectivity of photocatalytic-degradation of tetracycline hydrochloride[J].Environmental Science,2014,35(2):619-625.
[38]Jiang L,Hu X L,Yin D Q,et al.Occurrence,distribution and seasonal variation of antibiotics in the Huangpu river,Shanghai,China[J].Chemosphere,2011,82(6):822-828.
[39]Luo Y,Xu L,Rysz M,et al.Occurrence and transport of tetracycline,sulfonamide,quinolone,and macrolide antibiotics in the Haihe river basin,China[J].Environmental Science&Technology,2011,45(5):1827-1833.
[40]Sztaricskai F,Dinya Z,Batta G,et al.Chemical synthesis and structural study of lincomycin sulfoxides and a sulfone[J].The Journal of Antibiotics,1997,50(10):866-873.
[41]Wang C P,Ding Y J,Teppen B J,et al.Role of interlayer hydration in lincomycin sorption by smectite clays[J].Environmental Science&Technology,2009,43(16):6171-6176.
[42]张娣.磁性纳米Fe3O4去除水环境中抗生素类物质的研究[D].杨凌:西北农林科技大学,2011.
[43]Boursi B,Mamtani R,Haynes K,et al.Recurrent antibiotic exposure may promote cancer formation-another step in understanding the role of the human microbiota?[J].European Journal of Cancer,2015,51(17):2655-2664.
[2]甘秀梅,严清,高旭,等.典型抗生素在中国西南地区某污水处理厂中的行为和归趋[J].环境科学,2014,35(5):1817-1823.Gan X M,Yan Q,Gao X,et al.Occurrence and fate of typical antibiotics in a wastewater treatment plant in Southwest China[J].Environmental Science,2014,35(5):1817-1823.
[3]Watts C D,Craythorne M,Fielding M,et al.The 3rd European symposium on organic micropollutants[A].In:Angeletti G,Bjorseth A(Eds.).Analysis of Organic Micropollutants in Water.Dordrecht:Reidel Publishing Co.,1983.19-21.
[4]Homem V,Santos L.Degradation and removal methods of antibiotics from aqueous matrices-a review[J].Journal of Environmental Management,2011,92(10):2304-2347.
[5]Padhye L P,Yao H,Kung'u F T,et al.Year-long evaluation on the occurrence and fate of pharmaceuticals,personal care products,and endocrine disrupting chemicals in an urban drinking water treatment plant[J].Water Research,2014,51:266-276.
[6]Pruden A,Pei R T,Storteboom H,et al.Antibiotic resistance genes as emerging contaminants:studies in Northern Colorado[J].Environmental Science&Technology,2006,40(23):7445-7450.
[7]Sapkota A,Sapkota A R,Kucharski M,et al.Aquaculture practices and potential human health risks:current knowledge and future priorities[J].Environment International,2008,34(8):1215-1226.
[8]Luo Y,Mao D Q,Rysz M,et al.Trends in antibiotic resistance genes occurrence in the Haihe river,China[J].Environment Science&Technology,2010,44(19):7220-7225.
[9]Li N,Zhang X B,Wu W,et al.Occurrence,seasonal variation and risk assessment of antibiotics in the reservoirs in North China[J].Chemosphere,2014,111:327-335.
[10]阮悦斐,陈继淼,郭昌胜,等.天津近郊地区淡水养殖水体的表层水及沉积物中典型抗生素的残留分析[J].农业环境科学学报,2011,30(12):2586-2593.Ruan Y F,Chen J M,Guo C S,et al.Distribution characteristics of typical antibiotics in surface water and sediments from freshwater aquaculture water in Tianjin Suburban Areas,China[J].Journal of Agro-Environment Science,2011,30(12):2586-2593.
[11]徐琳,罗义,徐冰洁.海河底泥中12种抗生素残留的液相色谱串联质谱同时检测[J].分析测试学报,2010,29(1):17-21.Xu L,Luo Y,Xu B J.Simultaneous determination for 12antibiotics in sediments of Haihe River by HPLC-MS/MS method[J].Journal of Instrumental Analysis,2010,29(1):17-21.
[12]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,2016,37(12):4596-4604.Wu 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,2016,37(12):4596-4604.
[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,2016,37(7):2515-2521.Jin 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,2016,37(7):2515-2521.
[14]姜蕾,崔长征,黄岭.典型抗生素在饮用水厂的去除特征与健康风险[J].净水技术,2016,35(S1):100-103,121.)Jiang L,Cui C Z,Huang L.Removal of antibiotics in drinking water processes and their health risk[J].Water Purification Technology,2016,35(S1):100-103,121.
[15]Zhang X B,Guo W S,Ngo H H,et al.Performance evaluation of powdered activated carbon for removing 28 types of antibiotics from water[J].Journal of Environmental Management,2016,172:193-200.
[16]吴熊勋.城市水环境污染控制[M].南京:东南大学出版社,1989.
[17]王晨晨.城市家庭饮用水中三卤甲烷的健康风险评价方法研究[D].天津:天津大学,2013.
[18]张应华,刘志全,李广贺,等.基于不确定性分析的健康环境风险评价[J].环境科学,2007,28(7):1409-1415.Zhang Y H,Liu Z Q,Li G H,et al.Uncertainty analysis of health risk assessment caused by benzene contamination in a contaminated site[J].Environmental Science,2007,28(7):1409-1415.
[19]Crouch E,Wilson R.Regulation of carcinogens[J].Risk Analysis,1981,1(1):47-57.
[20]Zeise L,Wilson R,Crouch E.Use of acute toxicity to estimate carcinogenic risk[J].Risk Analysis,1984,4(3):187-199.
[21]Crouch E,Wilson R.Interspecies comparison of carcinogenic potency[J].Journal of Toxicology and Environmental Health,1979,5(6):1095-1118.
[22]Strenge D,Chamberlain P J.Multimedia environmental pollutant assessment system(MEPAs):exposure pathway and human health impact assessment models[M].Richland,WA:Pacific Northwest Laboratory,1995.
[23]Strenge D L,Peterson S R.Chemical data bases for the multimedia environmental pollutant assessment system(MEPAS):Version 1.[R].Richland,Washington:Pacific Northwest Lab.,1989.
[24]Layton D,Mallon B,Rosenblatt D,et al.Deriving allowable daily intakes for systemic toxicants lacking chronic toxicity data[J].Regulatory Toxicology and Pharmacology,1987,7(1):96-112.
[25]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.
[26]Dean R G.Compatibility of borrow material for beach fills[C].Coastal Engineering(1974).ASCE,2012.1319-1333.
[27]Zuccato E,Bagnati R,Fioretti F,et al.Environmental loads and detection of pharmaceuticals in Italy[A].In:Kümmerer K(Ed.).Pharmaceuticals in the Environment[M].Berlin Heidelberg:Springer,2001.19-27.
[28]崔亚丰,何江涛,苏思慧,等.某市典型地段地表水及地下水中氟喹诺酮类抗生素分布特征[J].环境科学,2015,36(11):4060-4067.Cui Y F,He J T,Su S H,et al.Distribution characteristics of fluoroquinolones antibiotics in surface water and groundwater from typical areas in a city[J].Environmental Science,2015,36(11):4060-4067.
[29]王冉,刘铁铮,王恬.抗生素在环境中的转归及其生态毒性[J].生态学报,2006,26(1):265-270.Wang R,Liu T Z,Wang T.The fate of antibiotics in environment and its ecotoxicology:a review[J].Acta Ecologica Sinica,2006,26(1):265-270.
[30]Qiao T J,Yu Z R,Zhang X H,et al.Occurrence and fate of pharmaceuticals and personal care products in drinking water in southern China[J].Journal of Environmental Monitoring,2011,13(11):3097-3103.
[31]Straub J O.Aquatic environmental risk assessment for human use of the old antibiotic sulfamethoxazole in Europe[J].Environmental Toxicology and Chemistry,2015,35(4):767-779.
[32]Dodd M C,Huang C H.Transformation of the antibacterial agent sulfamethoxazole in reactions with chlorine:kinetics,mechanisms,and pathways[J].Environmental Science&Technology,2004,38(21):5607-5615.
[33]Vieno N M,Hrkki H,Tuhkanen T,et al.Occurrence of pharmaceuticals in river water and their elimination in a pilotscale drinking water treatment plant[J].Environmental Science&Technology,2007,41(14):5077-5084.
[34]Li K X,Yediler A,Yang M,et al.Ozonation of oxytetracycline and toxicological assessment of its oxidation by-products[J].Chemosphere,2008,72(3):473-478.
[35]Turiel E,Bordin G,Rodríguez A R.Study of the evolution and degradation products of ciprofloxacin and oxolinic acid in river water samples by HPLC-UV/MS/MS-MS[J].Journal of Environmental Monitoring,2005,7(3):189-195.
[36]李耀中,孔欣,周岳溪,等.光催化降解三类难降解有机工业废水[J].中国给水排水,2003,19(1):5-8.Li Y Z,Kong X,Zhou Y X,et al.Photocatalytic degradation of three kinds of refractory industrial organic wastewater[J].China Water&Wastewater,2003,19(1):5-8.
[37]宋晨怡,尹大强.四环素光催化降解特性与选择性研究[J].环境科学,2014,35(2):619-625.Song C Y,Yin D Q.Characteristics and selectivity of photocatalytic-degradation of tetracycline hydrochloride[J].Environmental Science,2014,35(2):619-625.
[38]Jiang L,Hu X L,Yin D Q,et al.Occurrence,distribution and seasonal variation of antibiotics in the Huangpu river,Shanghai,China[J].Chemosphere,2011,82(6):822-828.
[39]Luo Y,Xu L,Rysz M,et al.Occurrence and transport of tetracycline,sulfonamide,quinolone,and macrolide antibiotics in the Haihe river basin,China[J].Environmental Science&Technology,2011,45(5):1827-1833.
[40]Sztaricskai F,Dinya Z,Batta G,et al.Chemical synthesis and structural study of lincomycin sulfoxides and a sulfone[J].The Journal of Antibiotics,1997,50(10):866-873.
[41]Wang C P,Ding Y J,Teppen B J,et al.Role of interlayer hydration in lincomycin sorption by smectite clays[J].Environmental Science&Technology,2009,43(16):6171-6176.
[42]张娣.磁性纳米Fe3O4去除水环境中抗生素类物质的研究[D].杨凌:西北农林科技大学,2011.
[43]Boursi B,Mamtani R,Haynes K,et al.Recurrent antibiotic exposure may promote cancer formation-another step in understanding the role of the human microbiota?[J].European Journal of Cancer,2015,51(17):2655-2664.