重庆主城区水域典型PhACs污染水平及生态风险评估
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摘要
采用固相萃取(SPE),高效液相色谱串联质谱法(HPLC-MSMS)检测分析了包括磺胺类、喹诺酮类、大环类酯类抗生素、心血管类、止痛剂类等8类PhACs(医药活性物质)在重庆主要地表水体长江、嘉陵江及花溪河的污染特征.结果表明,21种目标PhACs中,有14种在3条河流中均有检出,长江与嘉陵江的中ρ(PhACs)为1.1~35.5 ngL,花溪河ρ(PhACs)为10.3~445.6ngL.莫西沙星、苯扎贝特、吉非罗奇、双氯芬酸、阿托伐他汀等5种目标PhACs仅在花溪河中检出,质量浓度为0.6~31.4 ngL.氨氯地平未检出.花溪河流量小且周边污水直排严重,除磺胺甲嘧啶、立痛定与辛伐他汀外,其他目标PhACs的质量浓度显著高于其他2条河流.参照MECPNEC(MEC为环境实测浓度,PNEC为生态风险阈值)风险综合评估体系评估了水环境中PhACs的生态风险,在检测出的目标PhACs中,磺胺甲恶唑、氧氟沙星、红霉素、降固醇酸的生态风险熵(RQ=MECPNEC)均大于0.1,可能会对环境产生中等程度危害的生态风险,这与这4种PhACs的大量频繁使用密切相关.
The pollution characteristics of eight therapeutic groups,including antibiotics,analgesics,antiepileptics,antilipidemics,antihypersensitives,in the Yangtze River,Jialing River and Huaxi stream which is a tributary of the Yangtze River in Chongqing,were investigated using the high-performance liquid chromatography-electrospray ionization tandem mass spectrometry. Results showed that 14 of the 21 target PhACs were detected and the concentration levels ranged from 1. 1 to 35. 5 ng/L in the Yangtze River and Jialing River,while ranged from 10. 3 to 445. 6 ng/L in the Huaxi stream. Moxifloxacin,bezafibrate,gemfibrozil,diclofenac and atorvastatin were only detected in the Huaxi stream. The concentrations varied from 0. 6-31. 4 ng/L. Amlodipine was not found in this study. The flow of Huaxi stream is small and the direct emission of the surrounding sewage was very serious. Consequently,the concentrations of the target PhACs,except for sulfamethazine,carbamazepine and simvastatin,in Huaxi stream were statistically significantly higher than in the other two rivers. Risk quotients,the ratios of measured environmental concentrations( MEC) and the predicted no-effect concentrations,were over than 0. 1 for sulfamethoxazole, ofloxacin, erythromycin and clofibric acid,indicating that the environment concentrations of single compounds may have a medium ecological risk,which is closely related to their larger consumption.
The pollution characteristics of eight therapeutic groups,including antibiotics,analgesics,antiepileptics,antilipidemics,antihypersensitives,in the Yangtze River,Jialing River and Huaxi stream which is a tributary of the Yangtze River in Chongqing,were investigated using the high-performance liquid chromatography-electrospray ionization tandem mass spectrometry. Results showed that 14 of the 21 target PhACs were detected and the concentration levels ranged from 1. 1 to 35. 5 ng/L in the Yangtze River and Jialing River,while ranged from 10. 3 to 445. 6 ng/L in the Huaxi stream. Moxifloxacin,bezafibrate,gemfibrozil,diclofenac and atorvastatin were only detected in the Huaxi stream. The concentrations varied from 0. 6-31. 4 ng/L. Amlodipine was not found in this study. The flow of Huaxi stream is small and the direct emission of the surrounding sewage was very serious. Consequently,the concentrations of the target PhACs,except for sulfamethazine,carbamazepine and simvastatin,in Huaxi stream were statistically significantly higher than in the other two rivers. Risk quotients,the ratios of measured environmental concentrations( MEC) and the predicted no-effect concentrations,were over than 0. 1 for sulfamethoxazole, ofloxacin, erythromycin and clofibric acid,indicating that the environment concentrations of single compounds may have a medium ecological risk,which is closely related to their larger consumption.
引文
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[8]XU Weihai,ZHANG Gan,ZOU Shichan,et al.Determination of selected antibiotics in the Victoria Harbour and the Pearl River,South China using high-performance liquid chromatographyelectrospray ionization tandem mass spectrometry[J].Environ Pollut,2007,145(3):672-679.
[9]KARTHIKEYAN K G,MEYER M T.Occurrence of antibiotics in wastewater treatment facilities in Wisconsin,USA[J].Sci Total Environ,2006,361(1/2/3):196-207.
[10]KASPRZYK-HORDERN B,DINSDALE R M,GUWY A J.The occurrence of pharmaceuticals,personal care products,endocrine disruptors and illicit drugs in surface water in South Wales,UK[J].Water Res,2008,42(13):3498-3518.
[11]MIAO Xiusheng,BISHAY F,CHEN Mei.Occurrence of antimicrobials in the final effluents of wastewater treatment plants in Canada[J].Environ Sci Technol,2004,38(13):3533-3541.
[12]VRYZAS Z,ALEXOUDIS C,VASSILIOU G,et al.Determination and aquatic risk assessment of pesticide residues in riparian drainage canals in northeastern Greece[J].Ecotoxicol Environ Safety,2011,74(2):174-181.
[13]XU Weihai,ZHANG Gan,LI Xiangdong,et al.Occurrence and elimination of antibiotics at four sewage treatment plants in the Pearl River Delta(PRD),South China[J].Water Res,2007,41(19):4526-4534.
[14]GOBEL A,THOMSEN A,Mcardell C S,et al.Occurrence and sorption behavior of sulfonamides,macrolides,and trimethoprim in activated sludge treatment[J].Environ Sci Technol,2005,39(11):3981-3989.
[15]MCARDELL C S,MOLNAR E,SUTER M J,et al.Occurrence and fate of macrolide antibiotics in wastewater treatment plants and in the Glatt Valley watershed,Switzerland[J].Environ Sci Technol,2003,37(24):5479-5486.
[16]ZUCCATO E,BAGNATI R,FIORETTI F,et al.Environmental loads and detection of pharmaceuticals in Italy[M]//KMMERER K.Pharmaceuticals in the environment.Berlin:Springer,2001:19-27.
[17]HIRSCH R,TERNES T,HABERER K,et al.Occurrence of antibiotics in the aquatic environment[J].Sci Total Environ,1999,225(1/2):109-118.
[18]CHRISTIAN T,SCHNEIDER R J,FRBER H A,et al.Determination of antibiotic residues in manure,soil,and surface waters[J].Acta Hydrochimica Et Hydrobiologica,2003,31(1):36-44.
[19]BATT A L,BRUCE I B,AGA D S.Evaluating the vulnerability of surface waters to antibiotic contamination from varying wastewater treatment plant discharges[J].Environ Pollut,2006,142(2):295-302.
[20]WU Chenxi,WITTER J D,SPONGBERG AL,et al.Occurrence of selected pharmaceuticals in an agricultural landscape,western Lake Erie basin[J].Water Res,2009,43(14):3407-3416.
[21]BARTELT-HUNT S L,SNOW D D,DAMON T,et al.The occurrence of illicit and therapeutic pharmaceuticals in wastewater effluent and surface waters in Nebraska[J].Environ Pollut,2009,157(3):786-791.
[22]KOLPIN D W,FURLONG E T,MEYER M T,et al.Pharmaceuticals,hormones,and other organic wastewater contaminants in U.S.streams,1999-2000:a national reconnaissance[J].Environ Sci Technol,2002,36(6):1202-1211.
[23]ZUCCATO E,CASTIGLIONI S,BAGNATI R,et al.Source,occurrence and fate of antibiotics in the Italian aquatic environment[J].J Hazard Mater,2010,179(1/2/3):1042-1048.
[24]TAMTAM F,MERCIER F,LE BOT B,et al.Occurrence and fate of antibiotics in the Seine River in various hydrological conditions[J].Sci Total Environ,2008,393(1):84-95.
[25]GROS M,PETROVIC M,BARCELO D.Wastewater treatment plants as a pathway for aquatic contamination by pharmaceuticals in the Ebro River basin(Northeast Spain)[J].Environ Toxicol Chem,2007,26(8):1553-1562.
[26]PENG Xianzhi,YU Yiyi,TANG Caiming,et al.Occurrence of steroid estrogens,endocrine-disrupting phenols,and acid pharmaceutical residues in urban riverine water of the Pearl River Delta,South China[J].Sci Total Environ,2008,397(1/2/3):158-166.
[27]WANG Li,YING Guangguo,ZHAO Jianliang,et al.Occurrence and risk assessment of acidic pharmaceuticals in the Yellow River,Hai River and Liao River of north China[J].Sci Total Environ,2010,408(16):3139-3147.
[28]ZHAO Jianliang,YING Guoying,WANG Li,et al.Determination of phenolic endocrine disrupting chemicals and acidic pharmaceuticals in surface water of the Pearl Rivers in South China by gas chromatography-negative chemical ionization-mass spectrometry[J].Sci Total Environ,2009,407(2):962-974.
[29]CLEUVERS M.Aquatic ecotoxicity of pharmaceuticals including the assessment of combination effects[J].Toxicology Letters,2003,142(3):185-194.
[30]CLEUVERS M.Mixture toxicity of the anti-inflammatory drugs diclofenac,ibuprofen,naproxen,and acetylsalicylic acid[J].Ecotoxicol Environ Safety,2004,59(3):309-315.
[31]QUINN B,GAGNE F,BLAISE C.An investigation into the acute and chronic toxicity of eleven pharmaceuticals(and their solvents)found in wastewater effluent on the cnidarian,Hydra attenuata[J].Sci Total Environ,2008,389(2/3):306-314.
[32]TRIEBSKORN R,CASPER H,HEYD A,et al.Toxic effects of the non-steroidal anti-inflammatory drug diclofenac:partⅡ.cytological effects in liver,kidney,gills and intestine of rainbow trout(Oncorhynchus mykiss)[J].Aquatic Toxicology,2004,68(2):151-166.
[33]LOPEZ-SERNA R,POSTIGO C,BLANCO J,et al.Assessing the effects of tertiary treated wastewater reuse on the presence emerging contaminants in a Mediterranean river(Llobregat,NE Spain)[J].Environmental Science and Pollution Research,2012,19(4):1000-1012.
[34]KRASCSENITS Z,HILLER E,BARTAL M.Distribution of four human pharmaceuticals,carbamazepine,diclofenac,gemfibrozil,and ibuprofen between sediment and water[J].J Hydrol Hydromech,2008,56(4):237-246.
[35]GRUNG M,KALLQVIST T,SAKSHAUG S,et al.Environmental assessment of Norwegian priority pharmaceuticals based on the EMEA guideline[J].Ecotoxicol Environ Safety,2008,71(2):328-340.
[36]CHOI K,KIM Y,PARK J,et al.Seasonal variations of several pharmaceutical residues in surface water and sewage treatment plants of Han River,Korea[J].Sci Total Environ,2008,405(1/2/3):120-128.
[37]SANDERSON H,JOHNSON D J,WILSON C J,et al.Probabilistic hazard assessment of environmentally occurring pharmaceuticals toxicity to fish,daphnids and algae by ECOSAR screening[J].Toxicology Letters,2003,144(3):383-395.
[38]FERRARI B,MONS R,VOLLAT B,et al.Environmental risk assessment of six human pharmaceuticals:are the current environmental risk assessment procedures sufficient for the protection of the aquatic environment?[J]Environ Toxicol Chem,2004,23(5):1344-1354.
[39]YANG Lihua,YING Guangguo,SU Haochang,et al.Growthinhibiting effects of 12 antibacterial agents and their mixtures on the freshwater microalga Pseudokirchneriella subcapitata[J].Environ Toxicol Chem,2008,27(5):1201-1208.
[40]KHN R,PATTARD M,PERNAK K D,et al.Results of the harmful effects of water pollutants to Daphnia magna in the 21 day reproduction test[J].Water Res,1989,23(4):501-510.
[41]FLIPPIN J L,HUGGETT D,FORAN C M.Changes in the timing of reproduction following chronic exposure to ibuprofen in Japanese medaka,Oryzias latipes[J].Aquatic Toxicology,2007,81(1):73-78.
[42]HALLING-SORENSEN B.Algal toxicity of antibacterial agents used in intensive farming[J].Chemosphere,2000,40(7):731-739.
[43]HERNANDO M D,AGUERA A,FERNANDEZ-ALBA A R.LC-MS analysis and environmental risk of lipid regulators[J].Analytical and Bioanalytical Chemistry,2007,387(4):1269-1285.
[44]BOILLOT C.valuation des risquesécotoxicologiques liés aux rejets d'effluents hospitaliers dans les milieux aquatiques:contributionàl'amélioration de la phase“caratérisation des effets”[D].Lyon:Institut National des Sciences Appliquées,2008.
[45]关键.“超级阿斯匹林”——布洛芬(芬必得)的研发历史和在中国的发展[J].继续医学教育,2005,19(3):82-84.
[46]叶计朋,邹世春.典型抗生素类药物在珠江三角洲水体中的污染特征[J].生态环境,2007,16(2):384-388.
[2]LEUNG H W,MINH T B,MURPHY M B,et al.Distribution,fate and risk assessment of antibiotics in sewage treatment plants in Hong Kong,South China[J].Environ Intern,2012,42:1-9.
[3]VERLICCHI P,AUKIDY A M,ZAMBELLO E.Occurrence of pharmaceutical compounds in urban wastewater:removal,mass load and environmental risk after a secondary treatment:a review[J].Sci Total Environ,2012,429:123-155.
[4]GAO Panpan,MAO Dgqing,LUO Yi,et al.Occurrence of sulfonamide and tetracycline-resistant bacteria and resistance genes in aquaculture environment[J].Water Res,2012,46(7):2355-2364.
[5]ZHU Yongguan,JOHNSON T A,SU Jianqiang,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.
[6]KUMMERER K.Antibiotics in the aquatic environment:a review,part I[J].Chemosphere,2009,75(4):417-434.
[7]BUTTIGLIERI G,KNEPPER T P.Removal of emerging contaminants in wastewater treatment:conventional activated sludge treatment[M]//BARCELD,PETROVIC M.Emerging Contaminants from Industrial and Municipal Waste.Berlin:Springer,2008:1-35.
[8]XU Weihai,ZHANG Gan,ZOU Shichan,et al.Determination of selected antibiotics in the Victoria Harbour and the Pearl River,South China using high-performance liquid chromatographyelectrospray ionization tandem mass spectrometry[J].Environ Pollut,2007,145(3):672-679.
[9]KARTHIKEYAN K G,MEYER M T.Occurrence of antibiotics in wastewater treatment facilities in Wisconsin,USA[J].Sci Total Environ,2006,361(1/2/3):196-207.
[10]KASPRZYK-HORDERN B,DINSDALE R M,GUWY A J.The occurrence of pharmaceuticals,personal care products,endocrine disruptors and illicit drugs in surface water in South Wales,UK[J].Water Res,2008,42(13):3498-3518.
[11]MIAO Xiusheng,BISHAY F,CHEN Mei.Occurrence of antimicrobials in the final effluents of wastewater treatment plants in Canada[J].Environ Sci Technol,2004,38(13):3533-3541.
[12]VRYZAS Z,ALEXOUDIS C,VASSILIOU G,et al.Determination and aquatic risk assessment of pesticide residues in riparian drainage canals in northeastern Greece[J].Ecotoxicol Environ Safety,2011,74(2):174-181.
[13]XU Weihai,ZHANG Gan,LI Xiangdong,et al.Occurrence and elimination of antibiotics at four sewage treatment plants in the Pearl River Delta(PRD),South China[J].Water Res,2007,41(19):4526-4534.
[14]GOBEL A,THOMSEN A,Mcardell C S,et al.Occurrence and sorption behavior of sulfonamides,macrolides,and trimethoprim in activated sludge treatment[J].Environ Sci Technol,2005,39(11):3981-3989.
[15]MCARDELL C S,MOLNAR E,SUTER M J,et al.Occurrence and fate of macrolide antibiotics in wastewater treatment plants and in the Glatt Valley watershed,Switzerland[J].Environ Sci Technol,2003,37(24):5479-5486.
[16]ZUCCATO E,BAGNATI R,FIORETTI F,et al.Environmental loads and detection of pharmaceuticals in Italy[M]//KMMERER K.Pharmaceuticals in the environment.Berlin:Springer,2001:19-27.
[17]HIRSCH R,TERNES T,HABERER K,et al.Occurrence of antibiotics in the aquatic environment[J].Sci Total Environ,1999,225(1/2):109-118.
[18]CHRISTIAN T,SCHNEIDER R J,FRBER H A,et al.Determination of antibiotic residues in manure,soil,and surface waters[J].Acta Hydrochimica Et Hydrobiologica,2003,31(1):36-44.
[19]BATT A L,BRUCE I B,AGA D S.Evaluating the vulnerability of surface waters to antibiotic contamination from varying wastewater treatment plant discharges[J].Environ Pollut,2006,142(2):295-302.
[20]WU Chenxi,WITTER J D,SPONGBERG AL,et al.Occurrence of selected pharmaceuticals in an agricultural landscape,western Lake Erie basin[J].Water Res,2009,43(14):3407-3416.
[21]BARTELT-HUNT S L,SNOW D D,DAMON T,et al.The occurrence of illicit and therapeutic pharmaceuticals in wastewater effluent and surface waters in Nebraska[J].Environ Pollut,2009,157(3):786-791.
[22]KOLPIN D W,FURLONG E T,MEYER M T,et al.Pharmaceuticals,hormones,and other organic wastewater contaminants in U.S.streams,1999-2000:a national reconnaissance[J].Environ Sci Technol,2002,36(6):1202-1211.
[23]ZUCCATO E,CASTIGLIONI S,BAGNATI R,et al.Source,occurrence and fate of antibiotics in the Italian aquatic environment[J].J Hazard Mater,2010,179(1/2/3):1042-1048.
[24]TAMTAM F,MERCIER F,LE BOT B,et al.Occurrence and fate of antibiotics in the Seine River in various hydrological conditions[J].Sci Total Environ,2008,393(1):84-95.
[25]GROS M,PETROVIC M,BARCELO D.Wastewater treatment plants as a pathway for aquatic contamination by pharmaceuticals in the Ebro River basin(Northeast Spain)[J].Environ Toxicol Chem,2007,26(8):1553-1562.
[26]PENG Xianzhi,YU Yiyi,TANG Caiming,et al.Occurrence of steroid estrogens,endocrine-disrupting phenols,and acid pharmaceutical residues in urban riverine water of the Pearl River Delta,South China[J].Sci Total Environ,2008,397(1/2/3):158-166.
[27]WANG Li,YING Guangguo,ZHAO Jianliang,et al.Occurrence and risk assessment of acidic pharmaceuticals in the Yellow River,Hai River and Liao River of north China[J].Sci Total Environ,2010,408(16):3139-3147.
[28]ZHAO Jianliang,YING Guoying,WANG Li,et al.Determination of phenolic endocrine disrupting chemicals and acidic pharmaceuticals in surface water of the Pearl Rivers in South China by gas chromatography-negative chemical ionization-mass spectrometry[J].Sci Total Environ,2009,407(2):962-974.
[29]CLEUVERS M.Aquatic ecotoxicity of pharmaceuticals including the assessment of combination effects[J].Toxicology Letters,2003,142(3):185-194.
[30]CLEUVERS M.Mixture toxicity of the anti-inflammatory drugs diclofenac,ibuprofen,naproxen,and acetylsalicylic acid[J].Ecotoxicol Environ Safety,2004,59(3):309-315.
[31]QUINN B,GAGNE F,BLAISE C.An investigation into the acute and chronic toxicity of eleven pharmaceuticals(and their solvents)found in wastewater effluent on the cnidarian,Hydra attenuata[J].Sci Total Environ,2008,389(2/3):306-314.
[32]TRIEBSKORN R,CASPER H,HEYD A,et al.Toxic effects of the non-steroidal anti-inflammatory drug diclofenac:partⅡ.cytological effects in liver,kidney,gills and intestine of rainbow trout(Oncorhynchus mykiss)[J].Aquatic Toxicology,2004,68(2):151-166.
[33]LOPEZ-SERNA R,POSTIGO C,BLANCO J,et al.Assessing the effects of tertiary treated wastewater reuse on the presence emerging contaminants in a Mediterranean river(Llobregat,NE Spain)[J].Environmental Science and Pollution Research,2012,19(4):1000-1012.
[34]KRASCSENITS Z,HILLER E,BARTAL M.Distribution of four human pharmaceuticals,carbamazepine,diclofenac,gemfibrozil,and ibuprofen between sediment and water[J].J Hydrol Hydromech,2008,56(4):237-246.
[35]GRUNG M,KALLQVIST T,SAKSHAUG S,et al.Environmental assessment of Norwegian priority pharmaceuticals based on the EMEA guideline[J].Ecotoxicol Environ Safety,2008,71(2):328-340.
[36]CHOI K,KIM Y,PARK J,et al.Seasonal variations of several pharmaceutical residues in surface water and sewage treatment plants of Han River,Korea[J].Sci Total Environ,2008,405(1/2/3):120-128.
[37]SANDERSON H,JOHNSON D J,WILSON C J,et al.Probabilistic hazard assessment of environmentally occurring pharmaceuticals toxicity to fish,daphnids and algae by ECOSAR screening[J].Toxicology Letters,2003,144(3):383-395.
[38]FERRARI B,MONS R,VOLLAT B,et al.Environmental risk assessment of six human pharmaceuticals:are the current environmental risk assessment procedures sufficient for the protection of the aquatic environment?[J]Environ Toxicol Chem,2004,23(5):1344-1354.
[39]YANG Lihua,YING Guangguo,SU Haochang,et al.Growthinhibiting effects of 12 antibacterial agents and their mixtures on the freshwater microalga Pseudokirchneriella subcapitata[J].Environ Toxicol Chem,2008,27(5):1201-1208.
[40]KHN R,PATTARD M,PERNAK K D,et al.Results of the harmful effects of water pollutants to Daphnia magna in the 21 day reproduction test[J].Water Res,1989,23(4):501-510.
[41]FLIPPIN J L,HUGGETT D,FORAN C M.Changes in the timing of reproduction following chronic exposure to ibuprofen in Japanese medaka,Oryzias latipes[J].Aquatic Toxicology,2007,81(1):73-78.
[42]HALLING-SORENSEN B.Algal toxicity of antibacterial agents used in intensive farming[J].Chemosphere,2000,40(7):731-739.
[43]HERNANDO M D,AGUERA A,FERNANDEZ-ALBA A R.LC-MS analysis and environmental risk of lipid regulators[J].Analytical and Bioanalytical Chemistry,2007,387(4):1269-1285.
[44]BOILLOT C.valuation des risquesécotoxicologiques liés aux rejets d'effluents hospitaliers dans les milieux aquatiques:contributionàl'amélioration de la phase“caratérisation des effets”[D].Lyon:Institut National des Sciences Appliquées,2008.
[45]关键.“超级阿斯匹林”——布洛芬(芬必得)的研发历史和在中国的发展[J].继续医学教育,2005,19(3):82-84.
[46]叶计朋,邹世春.典型抗生素类药物在珠江三角洲水体中的污染特征[J].生态环境,2007,16(2):384-388.