尾水受纳河流中PhACs在传统水相中的分布及环境风险
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摘要
胶体介质不仅是水环境中污染物一个重要的"汇",还是污染物生物地球化学循环中至关重要的调控单元.本研究利用错流超滤、固相萃取、液相色谱质谱联用仪等前处理和分析检测方法调查了10种典型的药物活性化合物(PhACs)在污水厂尾水受纳河流传统水相中的分布和环境风险水平.结果表明,10种PhACs在水体溶解相和胶体中的含量分别达到27. 2～168. 1 ng·L~(-1)和164. 5～751. 1 ng·g~(-1).布洛芬(IPF)、罗红霉素(ROX)和红霉素(ETM)是两种介质中最为主要的污染物,三者污染浓度占到总浓度的80%以上.胶体对ROX、酮康唑、ETM和舍曲林都表现出较强的吸附性能,胶体/水分配系数(lg Kcol)在3. 2～4. 0之间,吸附率达到21. 1%～34. 5%. 10种PhACs对绿藻、溞和鱼的急、慢性毒性风险评估结果中,仅IPF对鱼类产生高等慢性风险,其余为中等风险及以下.值得注意的是,相对于急性风险来说,更多的PhACs对高等水生生物产生慢性不利影响.
Colloid media are not only an important " sink" for pollutants in the aquatic environment,but also a crucial regulating unit for the biogeochemical cycle of pollutants. In this study,the distribution and environmental risk levels of ten typical pharmaceutically active compounds( PhACs) in the water phase of effluent-receiving rivers were investigated using cross-flow ultrafiltration,solid-phase extraction,and liquid chromatography-tandem mass spectrometry as the pretreatment and analysis methods. The results showed that the total concentrations of the ten PhACs in the dissolved phase and colloidal phase ranged from 27. 2 to 168. 1 ng·L~(-1) and 164. 5 to 751. 1 ng·g~(-1),respectively. Ibuprofen( IPF),roxithromycin( ROX),and erythromycin( ETM) are the dominating pollutants in the dissolved phase and colloidal phase,accounting for more than 80% of the total concentration. Strong adsorption properties for ROX,ketoconazole,ETM,and sertraline were found in the colloid phase,their colloid/water distribution coefficients( lg Kcol) ranged from~3. 2 to 4. 0,and the percentage of PhACs absorbed to the colloidal phase reached 21. 1%-34. 5%. The risk assessment of acute and chronic toxicity to algae,daphnia,and fish showed that only IPF presented a high chronic risk to fish,while the risk levels of the other PhACs were at or below medium risk. It is worth noting that,in comparison with their acute risk,most PhACs have chronic negative effects on higher aquatic organisms.
Colloid media are not only an important " sink" for pollutants in the aquatic environment,but also a crucial regulating unit for the biogeochemical cycle of pollutants. In this study,the distribution and environmental risk levels of ten typical pharmaceutically active compounds( PhACs) in the water phase of effluent-receiving rivers were investigated using cross-flow ultrafiltration,solid-phase extraction,and liquid chromatography-tandem mass spectrometry as the pretreatment and analysis methods. The results showed that the total concentrations of the ten PhACs in the dissolved phase and colloidal phase ranged from 27. 2 to 168. 1 ng·L~(-1) and 164. 5 to 751. 1 ng·g~(-1),respectively. Ibuprofen( IPF),roxithromycin( ROX),and erythromycin( ETM) are the dominating pollutants in the dissolved phase and colloidal phase,accounting for more than 80% of the total concentration. Strong adsorption properties for ROX,ketoconazole,ETM,and sertraline were found in the colloid phase,their colloid/water distribution coefficients( lg Kcol) ranged from~3. 2 to 4. 0,and the percentage of PhACs absorbed to the colloidal phase reached 21. 1%-34. 5%. The risk assessment of acute and chronic toxicity to algae,daphnia,and fish showed that only IPF presented a high chronic risk to fish,while the risk levels of the other PhACs were at or below medium risk. It is worth noting that,in comparison with their acute risk,most PhACs have chronic negative effects on higher aquatic organisms.
引文
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[11]张盼伟,周怀东,赵高峰,等.北京城区水体中PPCPs的分布特征及潜在风险[J].环境科学,2017,38(5):1852-1862.Zhang P W,Zhou H D,Zhao G F,et al. Potential risk and distribution characteristics of PPCPs in surface water and sediment from rivers and lakes in Beijing, China[J].Environmental Science,2017,38(5):1852-1862.
[12] Liu J C,Lu G H,Xie Z X,et al. Occurrence,bioaccumulation and risk assessment of lipophilic pharmaceutically active compounds in the downstream rivers of sewage treatment plants[J]. Science of the Total Environment,2015,511:54-62.
[13]聂明华,晏彩霞,杨毅,等.黄浦江流域典型污水中不同粒径胶体的三维荧光光谱特征[J].环境科学,2017,38(8):3192-3199.Nie M H, Yan C X, Yang Y, et al. Fluorescence characterization of fractionated colloids in wastewaters received by Huangpu River[J]. Environmental Science,2017,38(8):3192-3199.
[14] Yan C X,Nie M H,Lead J R,et al. Application of a multimethod approach in characterization of natural aquatic colloids from different sources along Huangpu River in Shanghai,China[J]. Science of the Total Environment,2016,554-555:228-236.
[15] Yan C X,Nie M H,Yang Y,et al. Effect of colloids on the occurrence, distribution and photolysis of emerging organic contaminants in wastewaters[J]. Journal of Hazardous Materials,2015,299:241-248.
[16] Yan L Y,Zhang S H,Lin D,et al. Nitrogen loading affects microbes, nitrifiers and denitrifiers attached to submerged macrophyte in constructed wetlands[J]. Science of the Total Environment,2018,622-623:121-126.
[17] Duan Y P, Meng X Z, Wen Z H, et al. Multi-phase partitioning,ecological risk and fate of acidic pharmaceuticals in a wastewater receiving river:the role of colloids[J]. Science of the Total Environment,2013,447:267-273.
[18] Yang Y,Fu J,Peng H,et al. Occurrence and phase distribution of selected pharmaceuticals in the Yangtze Estuary and its coastal zone[J]. Journal of Hazardous Materials,2011,190(1-3):588-596.
[19] Cheng D M,Liu X H,Zhao S N,et al. Influence of the natural colloids on the multi-phase distributions of antibiotics in the surface water from the largest lake in North China[J]. Science of the Total Environment,2017,578:649-659.
[20] Liu J C, Dan X X, Lu G H, et al. Investigation of pharmaceutically active compounds in an urban receiving water:occurrence, fate and environmental risk assessment[J].Ecotoxicology and Environmental Safety, 2018, 154:214-220.
[21] Yan Z H, Yang H H, Dong HK, et al. Occurrence and ecological risk assessment of organic micropollutants in the lower reaches of the Yangtze River,China:a case study of water diversion[J]. Environmental Pollution,2018,239:223-232.
[22] Yan C X,Yang Y,Zhou J L,et al. Selected emerging organic contaminants in the Yangtze Estuary,China:a comprehensive treatment of their association with aquatic colloids[J]. Journal of Hazardous Materials,2015,283:14-23.
[23] 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.
[24] Ji Y,Wu P J,Zhang J,et al. Heavy metal accumulation,risk assessment and integrated biomarker responses of local vegetables:a case study along the Le'an river[J]. Chemosphere,2018,199:361-371.
[25] Han S, Choi K, Kim J, et al. Endocrine disruption and consequences of chronic exposure to ibuprofen in Japanese medaka(Oryzias latipes)and freshwater cladocerans Daphnia magna and Moina macrocopa[J]. Aquatic Toxicology,2010,98(3):256-264.
[26] Zuccato E, Castiglioni S, Fanelli R. Identification of the pharmaceuticals for human use contaminating the Italian aquatic environment[J]. Journal of Hazardous Materials,2005,122(3):205-209.
[2] Bu Q W,Wang B,Huang J,et al. Pharmaceuticals and personal care products in the aquatic environment in China:a review[J].Journal of Hazardous Materials,2013,262:189-211.
[3]温智皓,段艳平,孟祥周,等.城市污水处理厂及其受纳水体中5种典型PPCPs的赋存特征和生态风险[J].环境科学,2013,34(3):927-932.Wen Z H,Duan Y P,Meng X Z,et al. Occurrence and risk assessment of five selected PPCPs in municipal wastewater treatment plant and the receiving water[J]. Environmental Science,2013,34(3):927-932.
[4] Munz N A,Fu Q G,Stamm C,et al. Internal concentrations in gammarids reveal increased risk of organic micropollutants in wastewater-impacted streams[J]. Environmental Science&Technology,2018,52(18):10347-10358.
[5] Liu J L,Wong M H. Pharmaceuticals and personal care products(PPCPs):a review on environmental contamination in China[J]. Environment International,2013,59:208-224.
[6]张新波,宋姿,张丹,等.天津供水系统中抗生素分布变化特征与健康风险评价[J].环境科学,2018,39(1):99-108.Zhang X B,Song Z,Zhang D,et al. Distribution characteristics and health risk assessment of antibiotics in the water supply system in Tianjin[J]. Environmental Science,2018,39(1):99-108.
[7]陈晓雯,赵建亮,刘有胜,等.长江中下游环境激素效应的污染特征及生态风险[J].生态毒理学报,2016,11(3):191-203.Chen X W,Zhao J L,Liu Y S,et al. Occurrence and ecological risks of hormonal activities in the middle and lower reaches of Yangtze River[J]. Asian Journal of Ecotoxicology,2016,11(3):191-203.
[8] Biel-Maeso M,Baena-Nogueras R M,Corada-Fernández C,et al. Occurrence, distribution and environmental risk of pharmaceutically active compounds(PhACs)in coastal and ocean waters from the Gulf of Cadiz(SW Spain)[J]. Science of the Total Environment,2018,612:649-659.
[9] Burns E E,Carter L J,Kolpin D W,et al. Temporal and spatial variation in pharmaceutical concentrations in an urban river system[J]. Water Research,2018,137:72-85.
[10] Lin H J,Chen L L,Li H P,et al. Pharmaceutically active compounds in the Xiangjiang River,China:distribution pattern,source apportionment,and risk assessment[J]. Science of the Total Environment,2018,636:975-984.
[11]张盼伟,周怀东,赵高峰,等.北京城区水体中PPCPs的分布特征及潜在风险[J].环境科学,2017,38(5):1852-1862.Zhang P W,Zhou H D,Zhao G F,et al. Potential risk and distribution characteristics of PPCPs in surface water and sediment from rivers and lakes in Beijing, China[J].Environmental Science,2017,38(5):1852-1862.
[12] Liu J C,Lu G H,Xie Z X,et al. Occurrence,bioaccumulation and risk assessment of lipophilic pharmaceutically active compounds in the downstream rivers of sewage treatment plants[J]. Science of the Total Environment,2015,511:54-62.
[13]聂明华,晏彩霞,杨毅,等.黄浦江流域典型污水中不同粒径胶体的三维荧光光谱特征[J].环境科学,2017,38(8):3192-3199.Nie M H, Yan C X, Yang Y, et al. Fluorescence characterization of fractionated colloids in wastewaters received by Huangpu River[J]. Environmental Science,2017,38(8):3192-3199.
[14] Yan C X,Nie M H,Lead J R,et al. Application of a multimethod approach in characterization of natural aquatic colloids from different sources along Huangpu River in Shanghai,China[J]. Science of the Total Environment,2016,554-555:228-236.
[15] Yan C X,Nie M H,Yang Y,et al. Effect of colloids on the occurrence, distribution and photolysis of emerging organic contaminants in wastewaters[J]. Journal of Hazardous Materials,2015,299:241-248.
[16] Yan L Y,Zhang S H,Lin D,et al. Nitrogen loading affects microbes, nitrifiers and denitrifiers attached to submerged macrophyte in constructed wetlands[J]. Science of the Total Environment,2018,622-623:121-126.
[17] Duan Y P, Meng X Z, Wen Z H, et al. Multi-phase partitioning,ecological risk and fate of acidic pharmaceuticals in a wastewater receiving river:the role of colloids[J]. Science of the Total Environment,2013,447:267-273.
[18] Yang Y,Fu J,Peng H,et al. Occurrence and phase distribution of selected pharmaceuticals in the Yangtze Estuary and its coastal zone[J]. Journal of Hazardous Materials,2011,190(1-3):588-596.
[19] Cheng D M,Liu X H,Zhao S N,et al. Influence of the natural colloids on the multi-phase distributions of antibiotics in the surface water from the largest lake in North China[J]. Science of the Total Environment,2017,578:649-659.
[20] Liu J C, Dan X X, Lu G H, et al. Investigation of pharmaceutically active compounds in an urban receiving water:occurrence, fate and environmental risk assessment[J].Ecotoxicology and Environmental Safety, 2018, 154:214-220.
[21] Yan Z H, Yang H H, Dong HK, et al. Occurrence and ecological risk assessment of organic micropollutants in the lower reaches of the Yangtze River,China:a case study of water diversion[J]. Environmental Pollution,2018,239:223-232.
[22] Yan C X,Yang Y,Zhou J L,et al. Selected emerging organic contaminants in the Yangtze Estuary,China:a comprehensive treatment of their association with aquatic colloids[J]. Journal of Hazardous Materials,2015,283:14-23.
[23] 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.
[24] Ji Y,Wu P J,Zhang J,et al. Heavy metal accumulation,risk assessment and integrated biomarker responses of local vegetables:a case study along the Le'an river[J]. Chemosphere,2018,199:361-371.
[25] Han S, Choi K, Kim J, et al. Endocrine disruption and consequences of chronic exposure to ibuprofen in Japanese medaka(Oryzias latipes)and freshwater cladocerans Daphnia magna and Moina macrocopa[J]. Aquatic Toxicology,2010,98(3):256-264.
[26] Zuccato E, Castiglioni S, Fanelli R. Identification of the pharmaceuticals for human use contaminating the Italian aquatic environment[J]. Journal of Hazardous Materials,2005,122(3):205-209.
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