天津地区环境持久性药物污染物残留水平调查
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摘要
针对环境持久性药物污染物(EPPPs)的污染问题,采用固相萃取-高效液相色谱/串联质谱法,调查分析了22种环境持久性药物污染物在天津地区水体和沉积物中的残留水平和分布特征。结果显示,水源地水样中有19种EPPPs的检出率为100%,质量浓度范围为0.21～0.69μg·L~(-1),平均值为0.43μg·L~(-1)。地表水样中,除吉他霉素检出率为80%外,其余21种EPPPs的检出率均为100%,质量浓度范围为0.52～3.88μg·L~(-1),平均值为1.60μg·L~(-1)。沉积物样中共检出11种EPPPs,检出率为100%,含量范围为0.04～1.10μg·kg~(-1),平均值为0.52μg·kg~(-1)。其中蓟县于桥水库、蓟运河滨海新区段水样和独流减河滨海新区段沉积物样中检出的EPPPs残留水平较高,水体中环丙沙星、诺氟沙星与菲诺洛芬检出浓度较高,沉积物中则为吲哚美辛、水杨酸及氟苯尼考。对比国内外其他地区,天津地区水环境中EPPPs残留处于较高水平。
Accroding to the pollution problem of environmental persistent pharmaceutical pollutants(EPPPs), the residual levels and distribution characteristics of 22 kinds of environmental persistent pharmaceutical drug contaminants in water and sediments in Tianjin were investigated by solid phase extraction-high-performance liquid chromatography/tandem mass spectrometry. The results display that the detection rate of 19 kinds of EPPPs was 100% in the water samples from sources, and the concentration range and average concentration were 0.21-0.69 and 0.43 μg·L~(-1), respectively. As shown in the surface water samples except for kitasamycin(80%), the detection rate for other 21 kinds of EPPPs was all 100%. Moreover, the concentration range of these EPPPs was from 0.52 to 3.88 μg·L~(-1) and the average concentration was 1.60 μg·L~(-1). Furthermore, 11 kinds of EPPPs were detected completely(100%) in the sediments and the concentration range and average concentration were 0.04-1.10 and 0.52 μg·kg~(-1). Among the above results, the EPPPs residue levels of water samples in the Yuqiao reservoir of Jixian county, Jiyunhe of New Binhai section and sediments in the Duliujian river basin of New Binhai section were the highest. Compared with other EPPPs, the concentrations of ciprofloxacin, norfloxacin, fenoprofen in the water and indomethacin, salicylic acid, florfenicol in sediments were high. In summary, EPPPs residues level of water in Tianjin was higher than other regions in China and other countries.
Accroding to the pollution problem of environmental persistent pharmaceutical pollutants(EPPPs), the residual levels and distribution characteristics of 22 kinds of environmental persistent pharmaceutical drug contaminants in water and sediments in Tianjin were investigated by solid phase extraction-high-performance liquid chromatography/tandem mass spectrometry. The results display that the detection rate of 19 kinds of EPPPs was 100% in the water samples from sources, and the concentration range and average concentration were 0.21-0.69 and 0.43 μg·L~(-1), respectively. As shown in the surface water samples except for kitasamycin(80%), the detection rate for other 21 kinds of EPPPs was all 100%. Moreover, the concentration range of these EPPPs was from 0.52 to 3.88 μg·L~(-1) and the average concentration was 1.60 μg·L~(-1). Furthermore, 11 kinds of EPPPs were detected completely(100%) in the sediments and the concentration range and average concentration were 0.04-1.10 and 0.52 μg·kg~(-1). Among the above results, the EPPPs residue levels of water samples in the Yuqiao reservoir of Jixian county, Jiyunhe of New Binhai section and sediments in the Duliujian river basin of New Binhai section were the highest. Compared with other EPPPs, the concentrations of ciprofloxacin, norfloxacin, fenoprofen in the water and indomethacin, salicylic acid, florfenicol in sediments were high. In summary, EPPPs residues level of water in Tianjin was higher than other regions in China and other countries.
引文
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[17] 张君,程艳茹,封丽,等.三峡库区饮用水水源抗生素健康风险评价[J].环境科学与技术,2018,41(8):192-198.[ZHANG Jun,CHENG Yan-ru,FENG Li,et al.Health Risk Assessment of Antibiotics in the Centralized Drinking Water Source in the Three Gorges Reservoir Area[J].Environmental Science & Technology,2018,41(8):192-198.]
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[19] 徐浩,肖湘波,唐文浩,等.海口城区地表水环境中抗生素含量特征研究[J].环境科学与技术,2013,36(9):60-65.[XU Hao,XIAO Xiang-bo,TANG Wen-hao,et al.Concentration Characteristics of Antibiotics in Urban Aquatic Environment of Haikou[J].Environmental Science & Technology,2013,36(9):60-65.]
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[24] 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 Research,2008,42(13):3498-3518.
[25] CHITESCU C L,KAKLAMANOS G,NICOLAU A I,et al.High Sensitive Multiresidue Analysis of Pharmaceuticals and Antifungals in Surface Water Using U-HPLC-Q-Exactive Orbitrap HRMS.Application to the Danube River Basin on the Romanian Territory[J].Science of the Total Environment,2015,532:501-511.
[26] SZYMASKA U,WIERGOWSKI M,SO?TYSZEWSKI I,et al.Presence of Antibiotics in the Aquatic Environment in Europe and Their Analytical Monitoring:Recent Trends and Perspectives[J].Microchemical Journal,2019,147:729-740.
[2] CARBALLA M,OMIL F,LEMA J M,et al.Behavior of Pharmaceuticals,Cosmetics and Hormones in a Sewage Treatment Plant[J].Water Research,2004,38(12):2918-2926.
[3] 李红燕,陈兴汉.环境中抗生素的污染现状及危害[J].中国资源综合利用,2018,36(5):82-84,95.[LI Hong-yan,CHEN Xing-han.Pollution Status and Harm of Antibiotics in the Environment[J].China Resources Comprehensive Utilization,2018,36(5):82-84,95.]
[4] 关颖婷.基于LC-MS/MS检测潮海主要排污口和入海口32种药物的研究[D].大连:大连理工大学,2016.[GUAN Ying-ting.A LC-MS/MS Method Developed to Detect 32 Drugs in Water Sampled From Selected Drain Outlets and Estuaries of the Bohai Sea[D].Dalian:Dalian University of Technology,2016.]
[5] 高兴胜.UV/Na2S2O8降解污水中环境浓度非甾体抗炎药的研究[D].南京:南京大学,2018.[GAO Xing-sheng.Studies on the Degradation of Nonsteroidal Anti-Inflammatory Drugs at Environmental Concentration in Wastewater by UV/Na2S2O8[D].Nanjing:Nanjing University,2018.]
[6] SIM W J,LEE J W,LEE E S,et al.Occurrence and Distribution of Pharmaceuticals in Wastewater From Households,Livestock Farms,Hospitals and Pharmaceutical Manufactures[J].Chemosphere,2011,82(2):179-186.
[7] KUSTER M,LóPEZ DE ALDA M J,HERNANDO M D,et al.Analysis and Occurrence of Pharmaceuticals,Estrogens,Progestogens and Polar Pesticides in Sewage Treatment Plant Effluents,River Water and Drinking Water in the Llobregat River Basin(Barcelona,Spain)[J].Journal of Hydrology,2008,358(1/2):112-123.
[8] GRACIA-LOR E,SANCHO J V,SERRANO R,et al.Occurrence and Removal of Pharmaceuticals in Wastewater Treatment Plants at the Spanish Mediterranean Area of Valencia[J].Chemosphere,2012,87(5):453-462.
[9] 赵小光,赵仕海.蓟县于桥水库内源污染生物治理探讨[J].天津水产,2013(2):5-9.
[10] 王佳宁,徐永平,李晓宇,等.畜禽粪便抗生素残留及其对环境的影响[J].畜牧与兽医,2017,49(10):140-144.[WANG Jia-ning,XU Yong-ping,LI Xiao-yu,et al.Environmental Impact of Livestock and Poultry Manures With Antibiotic Residues[J].Animal Husbandry & Veterinary Medicine,2017,49(10):140-144.]
[11] 陈启华,孙静,王玉蕊.天津市蓟运河水系水环境问题及对策[J].低碳世界,2018(4):26-27.
[12] QIU W H,SUN J,FANG M J,et al.Occurrence of Antibiotics in the Main Rivers of Shenzhen,China:Association With Antibiotic Resistance Genes and Microbial Community[J].Science of The Total Environment.2019,653:334-341.
[13] 杨虹.独流减河水环境污染特征及生态风险评价研究[D].天津:天津工业大学,2017.
[14] 杭太俊.药物分析[M].7版.北京:人民卫生出版社,2015:198-200.[HANG Tai-jun.Medicine Analysis[M].7th ed.Beijing:People′s Health Publishing House,2015:198-200.]
[15] ZHENG W J,YOO K H,EL-ATY A M A,et al.Quantitative Determination of Carbasalate Calcium Derived Metabolites,Acetylsalicylic Acid and Salicylic Acid,in Six Animal Foods Using Liquid-Liquid Extraction Method Coupled With Liquid Chromatography-Tandem Mass Spectrometry[J].Food Chemistry,2019,278:744-750.
[16] 李涛,罗添允,罗玉洁,等.基于全羟基取代六元瓜环的固相微萃取搅拌棒对环境水样中非甾体抗炎药物的分析检测[J].药物分析杂志,2017,37(11):2062-2067.[LI Tao,LUO Tian-yun,LUO Yu-jie,et al.Determination of Non-Steroid Anti-Inflammatory Drugs in Environmental Water Samples by Stir Bar Sorptive Extraction Based on Perhydroxy Cucurbit[6] Uril[J].Chinese Journal of Pharmaceutical Analysis,2017,37(11):2062-2067.]
[17] 张君,程艳茹,封丽,等.三峡库区饮用水水源抗生素健康风险评价[J].环境科学与技术,2018,41(8):192-198.[ZHANG Jun,CHENG Yan-ru,FENG Li,et al.Health Risk Assessment of Antibiotics in the Centralized Drinking Water Source in the Three Gorges Reservoir Area[J].Environmental Science & Technology,2018,41(8):192-198.]
[18] 胡冠九,穆肃,赵永刚,等.南京典型县区饮用水源抗生素含量特征[J].环境化学,2015,34(1):192-193.]
[19] 徐浩,肖湘波,唐文浩,等.海口城区地表水环境中抗生素含量特征研究[J].环境科学与技术,2013,36(9):60-65.[XU Hao,XIAO Xiang-bo,TANG Wen-hao,et al.Concentration Characteristics of Antibiotics in Urban Aquatic Environment of Haikou[J].Environmental Science & Technology,2013,36(9):60-65.]
[20] 李文最,陈高水,郑艳影,等.闽江流域福州段水体中抗生素残留污染调查[J].实用预防医学,2018,25(12):1455-1458.[LI Wen-zui,CHEN Gao-shui,ZHENG Yan-ying,et al.Contamination Profiles of Antibiotics Residues in Water Bodies of the Fuzhou Section of the Minjiang River[J].Practical Preventive Medicine,2018,25(12):1455-1458.]
[21] PRAVEENA S M,SHAIFUDDIN S N M,SUKIMAN S,et al.Pharmaceuticals Residues in Selected Tropical Surface Water Bodies From Selangor (Malaysia):Occurrence and Potential Risk Assessments[J].Science of the Total Environment,2018,642:230-240.
[22] DA SILVA B F,JELIC A,LóPEZ-SERNA R,et al.Occurrence and Distribution of Pharmaceuticals in Surface Water,Suspended Solids and Sediments of the Ebro River Basin,Spain[J].Chemosphere,2011,85(8):1331-1339.
[23] MARSIK P,REZEK J,?IDKOVá M,et al.Non-Steroidal Anti-Inflammatory Drugs in the Watercourses of Elbe Basin in Czech Republic[J].Chemosphere,2017,171:97-105.
[24] 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 Research,2008,42(13):3498-3518.
[25] CHITESCU C L,KAKLAMANOS G,NICOLAU A I,et al.High Sensitive Multiresidue Analysis of Pharmaceuticals and Antifungals in Surface Water Using U-HPLC-Q-Exactive Orbitrap HRMS.Application to the Danube River Basin on the Romanian Territory[J].Science of the Total Environment,2015,532:501-511.
[26] SZYMASKA U,WIERGOWSKI M,SO?TYSZEWSKI I,et al.Presence of Antibiotics in the Aquatic Environment in Europe and Their Analytical Monitoring:Recent Trends and Perspectives[J].Microchemical Journal,2019,147:729-740.
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