典型城市污水中对羟基苯甲酸酯的污染特征
|
摘要
对羟基苯甲酸酯(parabens)作为防腐剂、防霉剂和杀菌剂等被广泛应用于食品、化妆品和药品中.近年来的研究表明,该类化合物能够在地表水体中检出,对水生生态环境存在潜在的危害.本研究于2016年秋季和冬季,对哈尔滨某典型城市污水处理厂进水进行了24 h连续采集,对6种parabens的质量浓度和4种常规水质指标进行了分析.结果表明,parabens普遍存在于城市污水中,对羟基苯甲酸甲酯、对羟基苯甲酸乙酯和对羟基苯甲酸丙酯是主要目标物,总有机碳、总溶解固体和酸碱度与parabens的浓度具有相关性;城市污水中parabens的质量浓度具有明显的日变化趋势,但是季节差异性不大.本研究结果为城市污水处理系统中parabens的深入研究和污染控制提供了重要理论依据.
Parabens are widely used in foodstuffs,cosmetics,and pharmaceuticals as preservatives,fungicides,and bactericides.Recent studies showed that these compounds could be detected in surface water and are a potential hazard to the aquatic ecological environment.In this study,24-hour influent samples were collected from a typical sewage wastewater treatment plant in Harbin in autumn and winter in 2016.The concentrations of six parabens and four normal water quality parameters were analyzed.The results indicated that parabens were frequently detected in the influent,and Me P,Et P,and Pr P were the predominant compounds.Significant correlations were found between TOC,TDS,pH,and the concentration of parabens.The concentration of parabens in the influent of the sewage wastewater treatment plant have obvious daily variations rather than seasonal variations.The results provide an important theoretical basis for further research and pollution control of parabens in sewage wastewater treatment system.
Parabens are widely used in foodstuffs,cosmetics,and pharmaceuticals as preservatives,fungicides,and bactericides.Recent studies showed that these compounds could be detected in surface water and are a potential hazard to the aquatic ecological environment.In this study,24-hour influent samples were collected from a typical sewage wastewater treatment plant in Harbin in autumn and winter in 2016.The concentrations of six parabens and four normal water quality parameters were analyzed.The results indicated that parabens were frequently detected in the influent,and Me P,Et P,and Pr P were the predominant compounds.Significant correlations were found between TOC,TDS,pH,and the concentration of parabens.The concentration of parabens in the influent of the sewage wastewater treatment plant have obvious daily variations rather than seasonal variations.The results provide an important theoretical basis for further research and pollution control of parabens in sewage wastewater treatment system.
引文
[1]林忠洋,马万里,齐迹,等.对羟基苯甲酸酯类防腐剂的人体暴露[J].化学进展,2015,27(5):614-622.Lin Z Y,Ma W L,Qi J,et al.Human exposure to parabens[J].Procress in Chemistry,2015,27(5):614-622.
[2]Soni M G,Carabin I G,Burdock G A.Safety assessment of esters of p-hydroxybenzoic acid(parabens)[J].Food and Chemical Toxicology,2005,43(7):985-1015.
[3]Darbre P D,Byford J R,Shaw L E,et al.Oestrogenic activity of isobutylparaben invitroand invivo[J].Journal of Applied Toxicology,2002,22(4):219-226.
[4]Lemini C,Jaimez R,ávila M E,et al.In vivo and in vitro estrogen bioactivities of alkyl parabens[J].Toxicology and Industrial Health,2003,19(2-6):69-79.
[5]Oishi S.Effects of butylparaben on the male reproductive system in rats[J].Toxicology and Industrial Health,2001,17(1):31-39.
[6]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.
[7]乔梦,齐维晓,赵旭,等.多环芳烃及其衍生物在北京典型污水处理厂中的存在及去除[J].环境科学,2016,37(4):1451-1459.Qiao M,Qi W X,Zhao X,et al.Occurrence and removal of polycyclic aromatic hydrocarbons and their derivatives in typical wastewater treatment plants in Beijing[J].Environmental Science,2016,37(4):1451-1459.
[8]张秋亚,马晓妍,王晓昌,等.典型生活污水处理工艺对雌激素效应的去除[J].环境科学,2017,38(4):1506-1512.Zhang Q Y,Ma X Y,Wang X C,et al.Removal of estrogenic effect by typical domestic wastewater treatment processes[J].Environmental Science,2017,38(4):1506-1512.
[9]Lee H B,Peart TE,Svoboda ML.Determination of endocrinedisrupting phenols,acidic pharmaceuticals,and personal-care products in sewage by solid-phase extraction and gas chromatography-mass spectrometry[J].Journal of Chromatography A,2005,1094(1-2):122-129.
[10]Blanco E,Casais MD C,Mejuto MC,et al.Combination of offline solid-phase extraction and on-column sample stacking for sensitive determination of parabens and p-hydroxybenzoic acid in waters by non-aqueous capillary electrophoresis[J].Analytica Chimica Acta,2009,647(1):104-111.
[11]Bratkowska D,MarcéR M,Cormack P A G,et al.Development and application of a polar coating for stir bar sorptive extraction of emerging pollutants from environmental water samples[J].Analytica Chimica Acta,2011,706(1):135-142.
[12]González-Mari1o I,Quintana JB,Rodríguez I,et al.Evaluation of the occurrence and biodegradation of parabens and halogenated by-products in wastewater by accurate-mass liquid chromatography-quadrupole-time-of-flight-mass spectrometry(LC-QTOF-MS)[J].Water Research,2011,45(20):6770-6780.
[13]Yu Y Y,Huang Q X,Wang Z F,et al.Occurrence and behavior of pharmaceuticals,steroid hormones,and endocrine-disrupting personal care products in wastewater and the recipient river water of the Pearl River Delta,South China[J].Journal of Environmental Monitoring,2011,13(4):871-878.
[14]Yu K,Li B,Zhang T.Direct rapid analysis of multiple PPCPs in municipal wastewater using ultrahigh performance liquid chromatography-tandem mass spectrometry without SPE preconcentration[J].Analytica Chimica Acta,2012,738:59-68.
[15]Sun Q,Li M Y,Ma C,et al.Seasonal and spatial variations of PPCP occurrence,removal and mass loading in three wastewater treatment plants located in different urbanization areas in Xiamen,China[J].Environmental Pollution,2016,208:371-381.
[16]Liao C Y,Chen L X,Kannan K.Occurrence of parabens in foodstuffs from China and its implications for human dietary exposure[J].Environment international,2013,57-58:68-74.
[17]Ma W L,Zhao X,Lin Z Y,et al.A survey of parabens in commercial pharmaceuticals from China and its implications for human exposure[J].Environment International,2016,95:30-35.
[18]Guo Y,Wang L,Kannan K.Phthalates and parabens in personal care products from China:concentrations and human exposure[J].Archives of Environmental Contamination and Toxicology,2014,66(1):113-119.
[19]Wang W,Kannan K.Fate of parabens and their metabolites in two wastewater treatment plants in New York State,United States[J].Environmental Science&Technology,2016,50(3):1174-1181.
[20]Karthikraj R,Vasu A K,Balakrishna K,et al.Occurrence and fate of parabens and their metabolites in five sewage treatment plants in India[J].Science of the Total Environment,2017,593-594:592-598.
[21]Eriksson E,Andersen H R,Madsen T S,et al.Greywater pollution variability and loadings[J].Ecological Engineering,2009,35(5):661-669.
[22]Gasperi J,Geara D,Lorgeoux C,et al.First assessment of triclosan,triclocarban and paraben mass loads at a very large regional scale:case of Paris conurbation(France)[J].Science of the Total Environment,2014,493:854-861.
[23]Chen Z F,Ying G G,Lai H J,et al.Determination of biocides in different environmental matrices by use of ultra-highperformance liquid chromatography-tandem mass spectrometry[J].Analytical and Bioanalytical Chemistry,2012,404(10):3175-3188.
[24]Carmona E,Andreu V,PicóY.Occurrence of acidic pharmaceuticals and personal care products in Turia River Basin:from waste to drinking water[J].Science of the Total Environment,2014,484:53-63.
[25]Loraine GA,Pettigrove ME.Seasonal variations in concentrations of pharmaceuticals and personal care products in drinking water and reclaimed wastewater in southern california[J].Environmental Science&Technology,2006,40(3):687-695.
[26]Canosa P,Rodríguez I,RubíE,et al.Optimisation of a solidphase microextraction method for the determination of parabens in water samples at the low ng per litre level[J].Journal of Chromatography A,2006,1124(1-2):3-10.
[27]Pedrouzo M,Borrull F,MarcéR M,et al.Ultra-highperformance liquid chromatography-tandem mass spectrometry for determining the presence of eleven personal care products in surface and wastewaters[J].Journal of Chromatography A,2009,1216(42):6994-7000.
[28]Kasprzyk-Hordern B,Dinsdale R M,Guwy A J.Multiresidue methods for the analysis of pharmaceuticals,personal care products and illicit drugs in surface water and wastewater by solid-phase extraction and ultra performance liquid chromatography-electrospray tandem mass spectrometry[J].Analytical and Bioanalytical Chemistry,2008,391(4):1293-1308.
[29]Kasprzyk-Hordern B,Dinsdale R M,Guwy A J.The removal of pharmaceuticals,personal care products,endocrine disruptors and illicit drugs during wastewater treatment and its impact on the quality of receiving waters[J].Water Research,2009,43(2):363-380.
[30]Andersen H R,Lundsbye M,Wedel H V,et al.Estrogenic personal care products in a greywater reuse system[J].Water Science and Technology,2007,56(12):45-49.
[31]Kusk K O,Krüger T,Long M H,et al.Endocrine potency of wastewater:contents of endocrine disrupting chemicals and effects measured by in vivo and in vitro assays[J].Environmental Toxicology and Chemistry,2011,30(2):413-426.
[32]Liao C Y,Liu F,Kannan K.Occurrence of and dietary exposure to parabens in foodstuffs from the United States[J].Environmental Science&Technology,2013,47(8):3918-3925.
[33]Moreta C,Tena M T,Kannan K.Analytical method for the determination and a survey of parabens and their derivatives in pharmaceuticals[J].Environmental Research,2015,142:452-460.
[2]Soni M G,Carabin I G,Burdock G A.Safety assessment of esters of p-hydroxybenzoic acid(parabens)[J].Food and Chemical Toxicology,2005,43(7):985-1015.
[3]Darbre P D,Byford J R,Shaw L E,et al.Oestrogenic activity of isobutylparaben invitroand invivo[J].Journal of Applied Toxicology,2002,22(4):219-226.
[4]Lemini C,Jaimez R,ávila M E,et al.In vivo and in vitro estrogen bioactivities of alkyl parabens[J].Toxicology and Industrial Health,2003,19(2-6):69-79.
[5]Oishi S.Effects of butylparaben on the male reproductive system in rats[J].Toxicology and Industrial Health,2001,17(1):31-39.
[6]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.
[7]乔梦,齐维晓,赵旭,等.多环芳烃及其衍生物在北京典型污水处理厂中的存在及去除[J].环境科学,2016,37(4):1451-1459.Qiao M,Qi W X,Zhao X,et al.Occurrence and removal of polycyclic aromatic hydrocarbons and their derivatives in typical wastewater treatment plants in Beijing[J].Environmental Science,2016,37(4):1451-1459.
[8]张秋亚,马晓妍,王晓昌,等.典型生活污水处理工艺对雌激素效应的去除[J].环境科学,2017,38(4):1506-1512.Zhang Q Y,Ma X Y,Wang X C,et al.Removal of estrogenic effect by typical domestic wastewater treatment processes[J].Environmental Science,2017,38(4):1506-1512.
[9]Lee H B,Peart TE,Svoboda ML.Determination of endocrinedisrupting phenols,acidic pharmaceuticals,and personal-care products in sewage by solid-phase extraction and gas chromatography-mass spectrometry[J].Journal of Chromatography A,2005,1094(1-2):122-129.
[10]Blanco E,Casais MD C,Mejuto MC,et al.Combination of offline solid-phase extraction and on-column sample stacking for sensitive determination of parabens and p-hydroxybenzoic acid in waters by non-aqueous capillary electrophoresis[J].Analytica Chimica Acta,2009,647(1):104-111.
[11]Bratkowska D,MarcéR M,Cormack P A G,et al.Development and application of a polar coating for stir bar sorptive extraction of emerging pollutants from environmental water samples[J].Analytica Chimica Acta,2011,706(1):135-142.
[12]González-Mari1o I,Quintana JB,Rodríguez I,et al.Evaluation of the occurrence and biodegradation of parabens and halogenated by-products in wastewater by accurate-mass liquid chromatography-quadrupole-time-of-flight-mass spectrometry(LC-QTOF-MS)[J].Water Research,2011,45(20):6770-6780.
[13]Yu Y Y,Huang Q X,Wang Z F,et al.Occurrence and behavior of pharmaceuticals,steroid hormones,and endocrine-disrupting personal care products in wastewater and the recipient river water of the Pearl River Delta,South China[J].Journal of Environmental Monitoring,2011,13(4):871-878.
[14]Yu K,Li B,Zhang T.Direct rapid analysis of multiple PPCPs in municipal wastewater using ultrahigh performance liquid chromatography-tandem mass spectrometry without SPE preconcentration[J].Analytica Chimica Acta,2012,738:59-68.
[15]Sun Q,Li M Y,Ma C,et al.Seasonal and spatial variations of PPCP occurrence,removal and mass loading in three wastewater treatment plants located in different urbanization areas in Xiamen,China[J].Environmental Pollution,2016,208:371-381.
[16]Liao C Y,Chen L X,Kannan K.Occurrence of parabens in foodstuffs from China and its implications for human dietary exposure[J].Environment international,2013,57-58:68-74.
[17]Ma W L,Zhao X,Lin Z Y,et al.A survey of parabens in commercial pharmaceuticals from China and its implications for human exposure[J].Environment International,2016,95:30-35.
[18]Guo Y,Wang L,Kannan K.Phthalates and parabens in personal care products from China:concentrations and human exposure[J].Archives of Environmental Contamination and Toxicology,2014,66(1):113-119.
[19]Wang W,Kannan K.Fate of parabens and their metabolites in two wastewater treatment plants in New York State,United States[J].Environmental Science&Technology,2016,50(3):1174-1181.
[20]Karthikraj R,Vasu A K,Balakrishna K,et al.Occurrence and fate of parabens and their metabolites in five sewage treatment plants in India[J].Science of the Total Environment,2017,593-594:592-598.
[21]Eriksson E,Andersen H R,Madsen T S,et al.Greywater pollution variability and loadings[J].Ecological Engineering,2009,35(5):661-669.
[22]Gasperi J,Geara D,Lorgeoux C,et al.First assessment of triclosan,triclocarban and paraben mass loads at a very large regional scale:case of Paris conurbation(France)[J].Science of the Total Environment,2014,493:854-861.
[23]Chen Z F,Ying G G,Lai H J,et al.Determination of biocides in different environmental matrices by use of ultra-highperformance liquid chromatography-tandem mass spectrometry[J].Analytical and Bioanalytical Chemistry,2012,404(10):3175-3188.
[24]Carmona E,Andreu V,PicóY.Occurrence of acidic pharmaceuticals and personal care products in Turia River Basin:from waste to drinking water[J].Science of the Total Environment,2014,484:53-63.
[25]Loraine GA,Pettigrove ME.Seasonal variations in concentrations of pharmaceuticals and personal care products in drinking water and reclaimed wastewater in southern california[J].Environmental Science&Technology,2006,40(3):687-695.
[26]Canosa P,Rodríguez I,RubíE,et al.Optimisation of a solidphase microextraction method for the determination of parabens in water samples at the low ng per litre level[J].Journal of Chromatography A,2006,1124(1-2):3-10.
[27]Pedrouzo M,Borrull F,MarcéR M,et al.Ultra-highperformance liquid chromatography-tandem mass spectrometry for determining the presence of eleven personal care products in surface and wastewaters[J].Journal of Chromatography A,2009,1216(42):6994-7000.
[28]Kasprzyk-Hordern B,Dinsdale R M,Guwy A J.Multiresidue methods for the analysis of pharmaceuticals,personal care products and illicit drugs in surface water and wastewater by solid-phase extraction and ultra performance liquid chromatography-electrospray tandem mass spectrometry[J].Analytical and Bioanalytical Chemistry,2008,391(4):1293-1308.
[29]Kasprzyk-Hordern B,Dinsdale R M,Guwy A J.The removal of pharmaceuticals,personal care products,endocrine disruptors and illicit drugs during wastewater treatment and its impact on the quality of receiving waters[J].Water Research,2009,43(2):363-380.
[30]Andersen H R,Lundsbye M,Wedel H V,et al.Estrogenic personal care products in a greywater reuse system[J].Water Science and Technology,2007,56(12):45-49.
[31]Kusk K O,Krüger T,Long M H,et al.Endocrine potency of wastewater:contents of endocrine disrupting chemicals and effects measured by in vivo and in vitro assays[J].Environmental Toxicology and Chemistry,2011,30(2):413-426.
[32]Liao C Y,Liu F,Kannan K.Occurrence of and dietary exposure to parabens in foodstuffs from the United States[J].Environmental Science&Technology,2013,47(8):3918-3925.
[33]Moreta C,Tena M T,Kannan K.Analytical method for the determination and a survey of parabens and their derivatives in pharmaceuticals[J].Environmental Research,2015,142:452-460.