宁波月湖水体中抗生素的分布与生态风险评价
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摘要
为探讨城市湖泊中抗生素的污染分布特征和生态风险,以宁波月湖为研究对象,利用固相萃取、超高效液相色谱-串联质谱法(HPLC-MS/MS)对月湖水体抗生素进行分析,并采用生态风险熵值法(RQ)和混合抗生素的风险法(MRQ)评价磺胺类、大环内酯类、喹诺酮类、β-内酰胺类、林可霉素(LIN)等10种抗生素的生态风险情况.结果表明:氨苄西林(AMS)的检出浓度最高,浓度变化范围在ND~382.0 ng/L;其次为头孢氨苄(LEX)、诺氟沙星(NOR)、磺胺间甲氧嘧啶(SMM)、LIN、阿奇霉素(AZM)、磺胺噻唑(STZ)、磺胺甲恶唑(SMX)、泰乐菌素(TYL)和磺胺嘧啶(SDZ),浓度范围分别为ND~283.0、ND~267.0、ND~219.0、31.50~209.0、ND~147.0、7.34~109.0、ND~104.0、ND~80.50和20.40~57.30 ng/L.月湖水体中10种目标抗生素的水平总体上高于自然湖泊,尤其β-内酰胺类和LIN在城市湖泊中广泛存在.生态风险评估的结果表明,LIN、TYL、SMX、NOR、AMS的生态风险值(RQ)值均大于1,具有高的生态风险;其余5种抗生素处于中或低的生态风险水平.本研究为城市湖泊抗生素生态风险问题的深入研究提供了一定的科学依据和基础.
The main objective of this study is focused on distribution characteristics,ecological risk assessment of selected antibiotics in the typical urban Moon Lake,which is situated in the center of Ningbo City. Water samples were concentrated by solid-phase extraction and determined by high-performance liquid chromatography-tandem mass spectrometry(HPLC-MS/MS). The environmental quotients posed by the selected antibiotics were assessed by using the methods of ecological risk quotients(RQ) and mixture risk quotients(MRQ). Composition analysis indicated that human-derived drugs significantly contributed to the total contamination of antibiotics in the lake. The ampicillin(AMS) was detected the highest concentration in the antibiotics and the range of concentration was ND to 382.0 ng/L. The maximum concentrations of cephalexin(LEX) and norfloxacin(NOR) were 283.0 ng/L and267.0 ng/L,respectively,which were relatively lower than AMS concentration levels. The detected concentration range of sulfamonomethoxine(SMM),lincomycin(LIN),azithromycin(AZM),sulfathiazole(STZ),sulfamethoxazole(SMX),tylosintartrate(TYL) and sulfadiazine(SDZ) were ND-219.0 ng/L,31.50-209.0 ng/L,ND-147.0 ng/L,7.34-109.0 ng/L,ND-104.0 ng/L,ND-80.50 ng/L and 20.40-57.30 ng/L,respectively. In comparison,the maximum concentration of most antibiotics in our investigated area were higher than natural lakes. The results of ecological risk assessment showed that the RQ values of LIN,TYL,SMX,NOR and AMS were higher than 1. That means these antibiotics have high ecological risks and the remaining five antibiotics are at lowor intermediate ecological risk. However,the calculated MRQ value for each sampling site was obviously higher than those from individual antibiotics,which suggested antibiotic mixtures could cause a higher detrimental effect to environment than individual antibiotic. This study will provide a scientific basis and foundation for the further study on the ecological risk of antibiotics in urban lakes.
The main objective of this study is focused on distribution characteristics,ecological risk assessment of selected antibiotics in the typical urban Moon Lake,which is situated in the center of Ningbo City. Water samples were concentrated by solid-phase extraction and determined by high-performance liquid chromatography-tandem mass spectrometry(HPLC-MS/MS). The environmental quotients posed by the selected antibiotics were assessed by using the methods of ecological risk quotients(RQ) and mixture risk quotients(MRQ). Composition analysis indicated that human-derived drugs significantly contributed to the total contamination of antibiotics in the lake. The ampicillin(AMS) was detected the highest concentration in the antibiotics and the range of concentration was ND to 382.0 ng/L. The maximum concentrations of cephalexin(LEX) and norfloxacin(NOR) were 283.0 ng/L and267.0 ng/L,respectively,which were relatively lower than AMS concentration levels. The detected concentration range of sulfamonomethoxine(SMM),lincomycin(LIN),azithromycin(AZM),sulfathiazole(STZ),sulfamethoxazole(SMX),tylosintartrate(TYL) and sulfadiazine(SDZ) were ND-219.0 ng/L,31.50-209.0 ng/L,ND-147.0 ng/L,7.34-109.0 ng/L,ND-104.0 ng/L,ND-80.50 ng/L and 20.40-57.30 ng/L,respectively. In comparison,the maximum concentration of most antibiotics in our investigated area were higher than natural lakes. The results of ecological risk assessment showed that the RQ values of LIN,TYL,SMX,NOR and AMS were higher than 1. That means these antibiotics have high ecological risks and the remaining five antibiotics are at lowor intermediate ecological risk. However,the calculated MRQ value for each sampling site was obviously higher than those from individual antibiotics,which suggested antibiotic mixtures could cause a higher detrimental effect to environment than individual antibiotic. This study will provide a scientific basis and foundation for the further study on the ecological risk of antibiotics in urban lakes.
引文
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[12] Li SJ,Dou HS,Shu JH et al. Water environmental problems of lakes and water ecosystem recovery in China. China Water Resources,2006,(13):14-17.[李世杰,窦鸿身,舒金华等.我国湖泊水环境问题与水生态系统修复的探讨.中国水利,2006,(13):14-17.]
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[14] Li W,Gao L,Shi Y et al. Occurrence,distribution and risks of antibiotics in urban surface water in Beijing,China. Environmental Science Processes&Impacts,2015,17(9):1611-1619.
[15] Tan F,Chen GY,Song W. Investigation on residues of antibiotics in lakes in Wuchang district of Wuhan City. Journal of Jianghan University:Natural Science Edition,2017,(5):406-410.[谭芳,陈高艺,宋威.武汉市武昌区湖泊中抗生素残留状况调查.江汉大学学报:自然科学版,2017,(5):406-410.]
[16] Zhang H,Du MM,Jiang HY et al. Occurrence,seasonal variation and removal efficiency of antibiotics and their metabolites in wastewater treatment plants,Jiulongjiang River Basin,South China. Environmental Science:Process&Impacts,2015,17(1):225-234.
[17] Verlicchi P,Aukidy AM,Galletti A et al. Hospital effluent:Investigation of the concentrations and distribution of pharmaceuticals and environmental risk assessment. Science of the Total Environment,2012,430:109-118.
[18] Li YX,Zhang XL,Li W et al. The residues and environmental risks of multiple veterinary antibiotics in animal faeces. Environmental Monitoring and Assessment,2013,185(3):2211-2220.
[19] Yan CX,Yang Y,Zhou JL et al. Antibiotics in the surface water of the Yangtze Estuary:Occurrence,distribution and risk assessment. Environmental Pollution,2013,175:22-29.
[20] Backhaus T,Faust M. Predictive environmental risk assessment of chemical mixtures:A conceptual framework. Environmental Science&Technology,2012,46(5):2564-2573.
[21] Liu JC,Lu GH,Xie ZX et al. Occurrence,bioaccumulation and risk assessment of lipophilic pharmaceutically active compounds in the downstream rivers of sewage treatment plants. Science of the Total Environment,2015,511:54-62.
[22] Yao LL,Wang YX,Tong L et al. Occurrence and risk assessment of antibiotics in surface water and groundwater from different depths of aquifers:A case study at Jianghan Plain,central China. Ecotoxicology and Environmental Safety,2017,135:236-242.
[23] Xue BM,Zhang RJ,Wang YH et al. Antibiotic contamination in a typical developing city in south China:Occurrence and ecological risks in the Yongjiang River impacted by tributary discharge and anthropogenic activities. Ecotoxicology and Environmental Safety,2013,92:229-236.
[24] U. S. Environmental Protection Agency. ECOTOX Database[DB/OL]. https://cfpub. epa. gov/ecotox/advanced_query.htm.
[25] 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? Environmental Toxicology and Chemistry,2004,23(5):1344-1354.
[26] Baran W,Sochacka J,Wardas W. Toxicity and biodegradability of sulfonamides and products of their photocatalytic degradation in aqueous solutions. Chemosphere,2006,65(8):1295-1299.
[27] Eguchi K,Nagase H,Ozawa M et al. Evaluation of antimicrobial agents for veterinary use in the ecotoxicity test using microalgae. Chemosphere,2004,57(11):1733-1738.
[28] Backhaus T,Scholze M,Grimme LH. The single substance and mixture toxicity of quinolones to the bioluminescent bacterium Vibrio fischeri. Aquatic Toxicology,2000,49(1):49-61.
[29] Kummerer K,Henninger A. Promoting resistance by the emission of antibiotics from hospitals and households into effluent.Clinical Microbiology and Infection,2003,9(12):1203-1214.
[30] Zhu TT,Song ZF,Duan BB et al. Research on pollution and health risk by anitibiotics in source water of Shiyan Reservoir in Shenzhen. Journal of Environment and Health,2013,30(11):1003-1006.[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.环境与健康杂志,2003,30(11):1003-1006.]
[31] Jank L,Hoff RB,Costa FJ et al. Simultaneous determination of eight antibiotics from distinct classes in surface and wastewater samples by solid-phase extraction and high-performance liquid chromatography-electrospray ionisation mass spectrometry. International Journal of Environmental Analytical Chemistry,2014,94(10):1013-1037.
[32] Xu J,Zhang Y,Zhou CB et al. Distribution,sources and composition of antibiotics in sediment,overlying water and pore water from Taihu Lake,China. Science of the Total Environment,2014,497:267-273.
[33] Liu X,Steele JC,Meng XZ. Usage,residue,and human health risk of antibiotics in Chinese aquaculture:A review. Environmental Pollution,2017,223:161-169.
[34] Xue Y,Chen YY. New development of cephalosporin antibiotics. Chinese Journal of Antibiotics,2011,(2):86-92.[薛雨,陈宇瑛.头孢菌素类抗生素的最新研究进展.中国抗生素杂志,2011,(2):86-92.]
[35] He X,Nie XJ,Ma YF et al. Advances of the preatment technology and residues ofβ-lactam antibiotics. Environmental Engineering,2017,35(9):145-149.[何欣,聂晓静,马洋帆等.β-内酰胺类抗生素前处理技术及其残留的研究进展.环境工程,2017,35(9):145-149.]
[36] Mandaric L,Dlamantini E,Stella E et al. Contamination sources and distribution patterns of pharmaceuticals and personal care products in Alpine rivers strongly affected by tourism. Science of the Total Environment,2017,590:484-494.
[37] Jiang AX,Li DQ,Xing HQ et al. Application of hydrolytic acidification—A biocontract oxidizing process for liquid-waste disposal. Journal of Safety and Environment,2002,2(2):3-6.[姜安玺,李德强,相会强等.水解酸化-生物接触氧化工艺在抗生素废水处理中的应用.安全与环境学报,2002,2(2):3-6.]
[38] Chang H,Hu JY,Wang LZ et al. Investigation of sulfonamides antibiotics in city sewage treatment plant. Chinese Science Bulletin,2008,53(2):159-164.[常红,胡建英,王乐征等.城市污水处理厂中磺胺类抗生素的调查研究.科学通报,2008,53(2):159-164.]
[39] Murata A,Takada H,Mutoh K et al. Nationwide monitoring of selected antibiotics:distribution and sources of sulfonamides,trimethoprim,and macrolides in Japanese rivers. Science of the Total Environment,2011,409(24):5305-5312.
[40] Wang QJ,Yi RH,Mo CH et al. The concentration characteristics of fluoroquinolone antibiotics in the aquatic environmental of Guangzhou. Ecological Science,2009,28(3):276-280.[王桥军,亦如瀚,莫测辉等.广州市水环境中喹诺酮类抗生素的污染特征.生态科学,2009,28(3):276-280.]
[2] Sharama VK,Johnson N,Cizmas L et al. A review of the influence of treatment strategies on antibiotic resistant bacteria and antibiotic resistance genes. Chemosphere,2016,150:702-714.
[3] Blair BD,Crago JP,Hedman CJ et al. Pharmaceuticals and personal care products found in the Great Lakes above concentrations of environmental concern. Chemosphere,2013,93(9):2116-2123.
[4] Chèvre N. Pharmaceuticals in surface waters:sources,behavior,ecological risk,and possible solutions. Case study of Lake Geneva,Switzerland. Wiley Interdisciplinary Reviews:Water,2014,1(1):69-86.
[5] Lin T,Yu S,Chen W. Occurrence,removal and risk assessment of pharmaceutical and personal care products(PPCPs)in an advanced drinking water treatment plant(ADWTP)around Taihu Lake in China. Chemosphere,2016,152:1-9.
[6] 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. Science of the Total Environment,2017,609:1423-1432.
[7] Ding HJ,Wu YX,Zhang WH et al. Occurrence,distribution,and risk assessment of antibiotics in the surface water of Poyang Lake,the largest freshwater lake in China. Chemosphere,2017,184:137-147.
[8] Cheng DM,Liu XH,Wang L et al. Seasonal variation and sediment-water exchange of antibiotics in a shallower large lake in North China. Science of the Total Environment,2014,476:266-275.
[9] Wu XY,Zou H,Zhu R et al. Occurrence,distribution and ecological risk of antibiotics in surface water of the Gonghu Bay,Taihu Lake. Environmental Science,2016,37(12):4596-4604.[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.环境科学,2016,37(12):4596-4604.]
[10] Yang Y,Cao X,Lin H et al. Antibiotics and antibiotic resistance genes in sediment of Honghu Lake and East Dongting Lake,China. Microbial Ecology,2016,72(4):791-801.
[11] Lei XN,Lu JJ,Liu ZL et al. Concentration and distribution of antibiotics in water-sediment system of Bosten Lake,Xinjiang. Environmental Science and Pollution Research,2015,22(3):1670-1678.
[12] Li SJ,Dou HS,Shu JH et al. Water environmental problems of lakes and water ecosystem recovery in China. China Water Resources,2006,(13):14-17.[李世杰,窦鸿身,舒金华等.我国湖泊水环境问题与水生态系统修复的探讨.中国水利,2006,(13):14-17.]
[13] Ding HJ,Zhong JY,Wu YX et al. Characteristics and ecological risk assessment of antibiotics in five city lakes in Nanchang City,Lake Poyang Catchment. J Lake Sci,2017,29(4):848-858. DOI:10.18307/2017.0408.[丁惠君,钟家有,吴亦潇等.鄱阳湖流域南昌市城市湖泊水体抗生素污染特征及生态风险分析.湖泊科学,2017,29(4):848-858.]
[14] Li W,Gao L,Shi Y et al. Occurrence,distribution and risks of antibiotics in urban surface water in Beijing,China. Environmental Science Processes&Impacts,2015,17(9):1611-1619.
[15] Tan F,Chen GY,Song W. Investigation on residues of antibiotics in lakes in Wuchang district of Wuhan City. Journal of Jianghan University:Natural Science Edition,2017,(5):406-410.[谭芳,陈高艺,宋威.武汉市武昌区湖泊中抗生素残留状况调查.江汉大学学报:自然科学版,2017,(5):406-410.]
[16] Zhang H,Du MM,Jiang HY et al. Occurrence,seasonal variation and removal efficiency of antibiotics and their metabolites in wastewater treatment plants,Jiulongjiang River Basin,South China. Environmental Science:Process&Impacts,2015,17(1):225-234.
[17] Verlicchi P,Aukidy AM,Galletti A et al. Hospital effluent:Investigation of the concentrations and distribution of pharmaceuticals and environmental risk assessment. Science of the Total Environment,2012,430:109-118.
[18] Li YX,Zhang XL,Li W et al. The residues and environmental risks of multiple veterinary antibiotics in animal faeces. Environmental Monitoring and Assessment,2013,185(3):2211-2220.
[19] Yan CX,Yang Y,Zhou JL et al. Antibiotics in the surface water of the Yangtze Estuary:Occurrence,distribution and risk assessment. Environmental Pollution,2013,175:22-29.
[20] Backhaus T,Faust M. Predictive environmental risk assessment of chemical mixtures:A conceptual framework. Environmental Science&Technology,2012,46(5):2564-2573.
[21] Liu JC,Lu GH,Xie ZX et al. Occurrence,bioaccumulation and risk assessment of lipophilic pharmaceutically active compounds in the downstream rivers of sewage treatment plants. Science of the Total Environment,2015,511:54-62.
[22] Yao LL,Wang YX,Tong L et al. Occurrence and risk assessment of antibiotics in surface water and groundwater from different depths of aquifers:A case study at Jianghan Plain,central China. Ecotoxicology and Environmental Safety,2017,135:236-242.
[23] Xue BM,Zhang RJ,Wang YH et al. Antibiotic contamination in a typical developing city in south China:Occurrence and ecological risks in the Yongjiang River impacted by tributary discharge and anthropogenic activities. Ecotoxicology and Environmental Safety,2013,92:229-236.
[24] U. S. Environmental Protection Agency. ECOTOX Database[DB/OL]. https://cfpub. epa. gov/ecotox/advanced_query.htm.
[25] 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? Environmental Toxicology and Chemistry,2004,23(5):1344-1354.
[26] Baran W,Sochacka J,Wardas W. Toxicity and biodegradability of sulfonamides and products of their photocatalytic degradation in aqueous solutions. Chemosphere,2006,65(8):1295-1299.
[27] Eguchi K,Nagase H,Ozawa M et al. Evaluation of antimicrobial agents for veterinary use in the ecotoxicity test using microalgae. Chemosphere,2004,57(11):1733-1738.
[28] Backhaus T,Scholze M,Grimme LH. The single substance and mixture toxicity of quinolones to the bioluminescent bacterium Vibrio fischeri. Aquatic Toxicology,2000,49(1):49-61.
[29] Kummerer K,Henninger A. Promoting resistance by the emission of antibiotics from hospitals and households into effluent.Clinical Microbiology and Infection,2003,9(12):1203-1214.
[30] Zhu TT,Song ZF,Duan BB et al. Research on pollution and health risk by anitibiotics in source water of Shiyan Reservoir in Shenzhen. Journal of Environment and Health,2013,30(11):1003-1006.[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.环境与健康杂志,2003,30(11):1003-1006.]
[31] Jank L,Hoff RB,Costa FJ et al. Simultaneous determination of eight antibiotics from distinct classes in surface and wastewater samples by solid-phase extraction and high-performance liquid chromatography-electrospray ionisation mass spectrometry. International Journal of Environmental Analytical Chemistry,2014,94(10):1013-1037.
[32] Xu J,Zhang Y,Zhou CB et al. Distribution,sources and composition of antibiotics in sediment,overlying water and pore water from Taihu Lake,China. Science of the Total Environment,2014,497:267-273.
[33] Liu X,Steele JC,Meng XZ. Usage,residue,and human health risk of antibiotics in Chinese aquaculture:A review. Environmental Pollution,2017,223:161-169.
[34] Xue Y,Chen YY. New development of cephalosporin antibiotics. Chinese Journal of Antibiotics,2011,(2):86-92.[薛雨,陈宇瑛.头孢菌素类抗生素的最新研究进展.中国抗生素杂志,2011,(2):86-92.]
[35] He X,Nie XJ,Ma YF et al. Advances of the preatment technology and residues ofβ-lactam antibiotics. Environmental Engineering,2017,35(9):145-149.[何欣,聂晓静,马洋帆等.β-内酰胺类抗生素前处理技术及其残留的研究进展.环境工程,2017,35(9):145-149.]
[36] Mandaric L,Dlamantini E,Stella E et al. Contamination sources and distribution patterns of pharmaceuticals and personal care products in Alpine rivers strongly affected by tourism. Science of the Total Environment,2017,590:484-494.
[37] Jiang AX,Li DQ,Xing HQ et al. Application of hydrolytic acidification—A biocontract oxidizing process for liquid-waste disposal. Journal of Safety and Environment,2002,2(2):3-6.[姜安玺,李德强,相会强等.水解酸化-生物接触氧化工艺在抗生素废水处理中的应用.安全与环境学报,2002,2(2):3-6.]
[38] Chang H,Hu JY,Wang LZ et al. Investigation of sulfonamides antibiotics in city sewage treatment plant. Chinese Science Bulletin,2008,53(2):159-164.[常红,胡建英,王乐征等.城市污水处理厂中磺胺类抗生素的调查研究.科学通报,2008,53(2):159-164.]
[39] Murata A,Takada H,Mutoh K et al. Nationwide monitoring of selected antibiotics:distribution and sources of sulfonamides,trimethoprim,and macrolides in Japanese rivers. Science of the Total Environment,2011,409(24):5305-5312.
[40] Wang QJ,Yi RH,Mo CH et al. The concentration characteristics of fluoroquinolone antibiotics in the aquatic environmental of Guangzhou. Ecological Science,2009,28(3):276-280.[王桥军,亦如瀚,莫测辉等.广州市水环境中喹诺酮类抗生素的污染特征.生态科学,2009,28(3):276-280.]