长三角某城镇典型小流域水体抗生素的污染分布特征
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摘要
为探讨城镇流域水体抗生素的污染分布特征,以宁波北仑芦江流域为研究对象,应用固相萃取、高效液相色谱-串联质谱法(HPLC-MS/MS)检测地表水中四环素类(TCs)、氯霉素类(CPs)、喹诺酮类(FQs)、大环内酯类(MLs)和磺胺类(SAs)5类抗生素的污染水平,分析其分布特征和可能的来源,并通过计算风险商进行生态风险评估。结果表明:芦江流域共有14种抗生素检出,其中TCs和CPs抗生素检出率和检出浓度最高;TCs抗生素检出率为96.9%,浓度范围为27.10~133.0 ng·L~(-1);CPs抗生素检出率为86.5%,浓度范围为13.00~219.0 ng·L~(-1)。TCs、CPs和FQs抗生素主要集中在农业区和工业区,污水排放为水体中抗生素的主要来源,包括农业源和工业源,以及生活源;MLs和SAs抗生素主要集中在生活区,相关污水来源主要为生活源。城市化程度较低的农业区抗生素浓度要高于城市化程度较高的工业区和生活区。生态风险评估结果显示,所检测出的抗生素处于高风险等级、中等风险等级、低风险等级、无风险等级的比例为5∶3∶3∶3,表明芦江流域部分水体中抗生素的污染具有较高的生态风险。
Solid-phase extraction(SPE)and high performance liquid chromatography tandem mass spectrometry(HPLC-MS/MS)were used to quantify five groups of antibiotics, which were tetracyclines(TCs), chloramphenicols(CPs), fluoroquinolones(FQs), macrolides(MLs),and sulfonamides(SAs), in the surface water of Lujiang River, Ningbo, a heavily industrialized and urbanized region in East China. The major aim of this study was to investigate the discharge of antibiotics, their potential distribution via non-point sources pollution(e.g. poultry farms), and the ecological risk to the river. A total of 14 antibiotics were detected in the surface water samples. The results indicated that the occurrence of antibiotic residues was widespread across the study site. Furthermore, TCs and CPs had the highest detection rates and concentration levels among the 14 antibiotics. The detection rate for TCs in the surface water reached 96.9% and the concentration range was from 27.10 ng·L~(-1) to 133.0 ng·L~(-1). The detection rate for CPs in the surface water reached 86.5% and the concentration range was from 13.00 ng·L~(-1) to 219.0 ng·L~(-1). The TCs, CPs, and FQs mainly occurred in the agricultural and industrial areas, and the non-point pollution sources were agricultural discharges, industrial wastewater, and domestic sewage. The MLs and SAs mainly occurred in domestic household areas, and the major non-point source was domestic sewage. The concentration of antibiotics in the domestic household area and the industrial area was lower than in the suburban agriculture area. Therefore, these results indicated that the antibiotic levels in the suburbs were higher than in the city area. The ecological risk assessment results showed that the risk of heavy, medium, low and safety pollution levels occurring were 5∶3∶3∶3. Therefore, the analyses undertaken in this study suggested that approximately 50.0% of the areas had a high ecological risk due to antibiotics.
Solid-phase extraction(SPE)and high performance liquid chromatography tandem mass spectrometry(HPLC-MS/MS)were used to quantify five groups of antibiotics, which were tetracyclines(TCs), chloramphenicols(CPs), fluoroquinolones(FQs), macrolides(MLs),and sulfonamides(SAs), in the surface water of Lujiang River, Ningbo, a heavily industrialized and urbanized region in East China. The major aim of this study was to investigate the discharge of antibiotics, their potential distribution via non-point sources pollution(e.g. poultry farms), and the ecological risk to the river. A total of 14 antibiotics were detected in the surface water samples. The results indicated that the occurrence of antibiotic residues was widespread across the study site. Furthermore, TCs and CPs had the highest detection rates and concentration levels among the 14 antibiotics. The detection rate for TCs in the surface water reached 96.9% and the concentration range was from 27.10 ng·L~(-1) to 133.0 ng·L~(-1). The detection rate for CPs in the surface water reached 86.5% and the concentration range was from 13.00 ng·L~(-1) to 219.0 ng·L~(-1). The TCs, CPs, and FQs mainly occurred in the agricultural and industrial areas, and the non-point pollution sources were agricultural discharges, industrial wastewater, and domestic sewage. The MLs and SAs mainly occurred in domestic household areas, and the major non-point source was domestic sewage. The concentration of antibiotics in the domestic household area and the industrial area was lower than in the suburban agriculture area. Therefore, these results indicated that the antibiotic levels in the suburbs were higher than in the city area. The ecological risk assessment results showed that the risk of heavy, medium, low and safety pollution levels occurring were 5∶3∶3∶3. Therefore, the analyses undertaken in this study suggested that approximately 50.0% of the areas had a high ecological risk due to antibiotics.
引文
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[2]Zhang Q Q,Ying G G,Pan C G,et al.A comprehensive evaluation of antibiotics emission and fate in the river basins of China:Source analysis,multimedia modelling,and linkage to bacterial resistance[J].Environment science&Technology,2015,49(11):6772-6782.
[3]Kummerer K.Antibiotics in the aquatic environment:A review-Part I[J].Chemosphere,2009,75(4):417-434.
[4]Zhu Y G,Johnson T A,Su J Q,et al.Diverse and abundant antibiotic resistance genes in Chinese swine farms[J].Proceedings of the National Academy of Sciences of the United States of America,2013,110(9):3435-3440.
[5]朱婷婷,宋战锋,段标标,等.深圳石岩水库抗生素污染特征与健康风险初步评价[J].环境与健康杂志,2013,30(11):107-110.ZHU Ting-ting,SONG Zhan-feng,DUAN Biao-biao,et al.Research on pollution and health risk by antibiotics in source water of Shiyan Reservoir in Shenzhen[J].Journal of Environment and Health,2013,30(11):107-110.
[6]Kolpin D W,Furlong E T,Meyer M T,et al.Pharmaceuticals,hormones,and other organic wastewater contaminants in US streams,1999—2000:A national reconnaissance[J].Environmental Science&Technology,2002,36(6):1202-1211.
[7]Watkinson A J,Murby E J,Kolpin D W,et al.The occurrence of antibiotics in an urban watershed:From wastewater to drinking water[J].Science of the Total Environment,2009,407(8):2711-2723.
[8]Jiang Y H,Li M X,Guo C S,et al.Distribution and ecological risk of antibiotics in a typical effluent-receiving river(Wangyang River)in North China[J].Chemosphere,2014,112:267-274.
[9]Zhang D D,Lin L F,Luo Z X,et al.Occurrence of selected antibiotics in Jiulongjiang River in various seasons,South China[J].Journal of Environmental Monitoring,2011,13(7):1953-1960.
[10]Sun Q,Li Y,Li M Y,et al.PPCPs in Jiulong River estuary(China):Spatiotemporal distributions,fate,and their use as chemical markers of wastewater[J].Chemosphere,2016,150:596-604.
[11]Yang J F,Ying G G,Zhao J L,et al.Spatial and seasonal distribution of selected antibiotics in surface waters of the Pearl Rivers,China[J].Journal of Environmental Science and Health Part B-Pesticides Food Contaminants and Agricultural Wastes,2011,46(3):272-280.
[12]武旭跃,邹华,朱荣,等.太湖贡湖湾水域抗生素污染特征分布和生态风险评价[J].环境科学,2016,37(12):4596-4604.WU Xu-yue,ZOU Hua,ZHU Rong,et al.Occurrence,distribution and ecological risk of antibiotics in surface water of the Gonghu Bay,Taihu Lake[J].Environment Science,2016,37(12):4596-4604.
[13]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.
[14]Xu W H,Zhang G,Zou S C,et al.A preliminary investigation on the occurrence and distribution of antibiotics in the Yellow River and its tributaries,China[J].Water Environment Research,2009,81(3):248-254.
[15]Yan C X,Yang Y,Zhou J L,et al.Antibiotics in the surface water of the Yangtze Estuary:Occurrence,distribution and risk assessment[J].Environmental Pollution,2013,175:22-29.
[16]Xu Y,Guo C S,Luo Y,et al.Occurrence and distribution of antibiotics,antibiotic resistance genes in the urban rivers in Beijing,China[J].Environmental Pollution,2016,213:833-840.
[17]Wang Z,Zhang X H,Huang Y,et al.Comprehensive evaluation of pharmaceuticals and personal care products(PPCPs)in typical highly urbanized regions across China[J].Environmental Pollution,2015,204:223-232.
[18]Chen H,Li X J,Zhu S C.Occurrence and distribution of selected pharmaceuticals and personal care products in a aquatic environments:A comparative study of regions in China with different urbanization levels[J].Environmental Science and Pollution Research,2012,19(6):2381-2389.
[19]中华人民共和国国家统计局.中国统计年鉴2011[DB/OL].[2017-11-27].http://www.stats.gov.cn/tjsj/ndsj/2011/indexch.htm.National Bureau of Statistics of the People′s Republic of China:China statistical yearbook[DB/OL].[2017-11-27].http://www.stats.gov.cn/tjsj/ndsj/2011/indexch.htm.
[20]李嘉,张瑞杰,王润梅,等.小清河流域抗生素污染分布特征和生态风险评估[J].农业环境科学学报,2016,35(7):1384-1391.LI Jia,ZHANG Rui-jie,WANG Run-mei,et al.Distribution characteristics and ecological risk assessment of antibiotic pollution in Xiaoqing River watershed[J].Journal of Agro-Environment Science,2016,35(7):1384-1391.
[21]Kim S C,Carlson K.Temporal and spatial trends in the occurrence of human and veterinary antibiotics in aqueous and river sediment matrices[J].Environmental Science&Technology,2007,41(1):50-57.
[22]赵腾辉,陈奕涵,韩巍,等.东江上游典型抗生素污染特征及生态风险评价[J].生态环境学报,2016,25(10):1707-1713.ZHAO Teng-hui,CHEN Yi-han,HAN Wei,et al.The contamination characteristics and ecological risk assessment of typical antibiotics in the upper reaches of the Dongjiang River[J].Ecology and Environmental Sciences,2016,25(10):1707-1713.
[23]Sun Q,Lv M,Hu A Y,et al.Seasonal variation in the occurrence and removal of pharmaceuticals and personal care products in a wastewater treatment plant in Xiamen,China[J].Journal of Hazardous Materials,2014,277:69-75.
[24]Dai G H,Wang B,Fu C C,et al.Pharmaceuticals and personal care products(PPCPs)in urban and suburban rivers of Beijing,China:Occurrence,source apportionment and potential ecological risk[J].Environmental Science-processes&Impacts,2016,18(4):445-455.
[25]Zhang H,Du M M,Jiang H Y,et al.Occurrence,seasonal variation and removal efficiency of antibiotics and their metabolites in wastewater treatment plants,Jiulongjiang River Basin,South China[J].Environmental Science-Processes&Impacts,2015,17(1):225-234.
[26]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.
[27]Yang L,He J T,Su S H,et al.Occurrence,distribution,and attenuation of pharmaceuticals and personal care products in the riverside groundwater of the Beiyun River of Beijing,China[J].Environmental Science and Pollution Research,2017,24(18):15838-15851.
[28]Chen H X,Chen H,Ying J,et al.Dispersive liquid-liquid microextraction followed by high-performance liquid chromatography as an efficient and sensitive technique for simultaneous determination of chloramphenicol and thiamphenicol in honey[J].Analytica Chimica Acta,2009,632(1):80-85.
[29]Gantverg A,Shishani I,Hoffman M.Determination of chloramphenicol in animal tissues and urine-liquid chromatography-tandem mass spectrometry versus gas chromatography-mass spectrometry[J].Analytica Chimica Acta,2003,483(1/2):125-135.
[30]Xu W H,Zhang G,Zou S C,et al.Determination of selected antibiotics in the Victoria Harbour and the Pearl River,South China using highperformance liquid chromatography-electrospray ionization tandem mass spectrometry[J].Environmental Pollution,2007,145(3):672-679.
[31]Doll T E,Frimmel F H.Fate of pharmaceuticals-photodegradation by simulated solar UV-light[J].Chemosphere,2003,52(10):1757-1769.
[32]Lunestad B T,Samuelsen O B,Fjelde S,et al.Photostability of eight antibacterial agents in seawater[J].Aquaculture,1995,134(3/4):217-225.
[33]Castiglioni S,Bagnati R,Fanelli R,et al.Removal of pharmaceuticals in sewage treatment plants in Italy[J].Environmental Science&Technology,2006,40(1):357-363.
[34]Stepanic V,Ziher D,Gabelica M,et al.Physicochemical profile of macrolides and their comparison with small molecules[J].European Journal of Medicinal Chemistry,2012,47:462-472.
[35]Murata A,Takada H,Mutoh K,et al.Nationwide monitoring of selected antibiotics:Distribution and sources of sulfonamides,trimethoprim,and macrolides in Japanese rivers[J].Science of the Total Environment,2011,409(24):5305-5312.
[36]Huang C H,Renew J E,Smeby K L,et al.Assessment of potential antibiotic contaminants in water and preliminary occurrence analysis[J].Water Resources Update,2001,120:334-342.
[37]葛林科.水中溶解性物质对氯霉素类和氟喹诺酮类抗生素光降解的影响[D].大连:大连理工大学,2009.GE Lin-ke.Effects of aqueous dissolved matter on photodegradation of phenicol and fluoroquinolone antibiotics[D].Dalian:Dalian University of Technology,2009.
[38]Pouliquen H,Delpepee R,Larhantec-Verdier M,et al.Comparative hydrolysis and photolysis of four antibacterial agents(oxytetracycline oxolinic acid,flumequine and florfenicol)in deionised water,freshwater and seawater under abilotic conditions[J].Aquaculture,2007,262(1):23-28.
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