汾河沿岸农田土壤喹诺酮类抗生素残留特征及风险评估
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摘要
选取山西省汾河沿岸71个代表性农田土壤,采用液相色谱-质谱联用法(LC-MS/MS)分析了4种喹诺酮类抗生素(quinolones,QLs)的残留水平和空间分布特征,探究影响抗生素残留的环境因子,并评估QLs残留的生态风险.结果表明:①汾河沿岸农田土壤中QLs检出情况为:诺氟沙星(norfloxacin,NFC)、环丙沙星(ciprofloxacin,CFC)、恩氟沙星(enrofloxacin,EFC)检出率为100%,氧氟沙星(ofloxacin,OFC)检出率为98.6%,QLs分布广泛.土壤样品中QLs组成以NFC为主,平均检出浓度为2.54μg·kg~(-1),其次为CFC和OFC,平均检出浓度分别为0.54μg·kg~(-1)和0.36μg·kg~(-1).②空间分布特征分析表明,上中游QLs检出情况相似,均表现为EFC Seventy-one representative samples of farmland soil were collected along the Fenhe River in Shanxi, to understand the residue characteristics of four kinds of quinolones, analyze the effect from environmental factors on residual antibiotics, and evaluate the ecological risk. The results revealed that: ①QLs distributed widely along the Fenhe River. Enrofloxacin(EFC), ciprofloxacin(CFC) and norfloxacin(NFC) were detected in all samples, and the detection rate of ofloxacin(OFC) was 98.6%. The concentration of NFC was the highest(2.54 μg·kg~(-1)), followed by OFC and CFC, whose average concentrations were 0.36 μg·kg~(-1) and 0.54 μg·kg~(-1), respectively. ②The spatial distribution characteristics of the upstream and midstream showed as EFC < OFC < CFC < NFC, while that in the downstream has converted to EFC < CFC < OFC < NFC. The antibiotic had relatively high concentrations in soil along the midstream of the Fenhe River. The antibiotic concentration in Qingxu County was the highest(19.67 μg·kg~(-1)), followed by Lingshi County(15.21 μg·kg~(-1)), which should be taken into consideration seriously. ③QLs were negatively correlated with pH. NFC, CFC and EFC were poorly correlated with organic matter content, while OFC was positively correlated, which might be related to the hydrogen bond between oxygen and polar functional groups of organic matter. NFC, CFC and EFC were positively correlated with the cation exchange capacity(CEC), while OFC was absent correlated, which might be related to the weak force of weakly polar epoxy ether. NFC and OFC were positively correlated with the soil sand content. ④The ecological risks of QLs were rlatively low, among which NFC, OFC and CFC presented moderate and low risks, while EFC presented low risk. This study aims to provide scientific basis for QLs pollution control and agricultural product safety supervision along the Fenhe River.
引文
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Briones R M,Sarmah A K,Padhye L P.2016.A global perspective on the use,occurrence,fate and effects of anti-diabetic drug metformin in natural and engineered ecosystems[J].Environmental Pollution,219:1007-1020
Bruchet A,Hochereau C,Picard C,et al.2005.Analysis of drugs and personal care products in French source and drinking waters:the analytical challenge and examples of application[J].Water Science& Technology,52(8):53-61
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冯佳,郭宇宁,王飞,等.2016.太原汾河景区浮游植物群落结构及其与环境因子关系分析[J].环境科学,37(4):1353-1361
Gong W,Liu X,He H,et al.2012.Quantitatively modeling soil-water distribution coefficients of three antibiotics using soil physicochemical properties[J].Chemosphere,89(7):825-831
Grenni P,Ancona V,Barra A.2017.Ecological effects of antibiotics on natural ecosystems:A review[J].Microchemical Journal,136:25-39
管荷兰,于海凤,王嘉宇.2012.氟喹诺酮类抗生素在土壤中的归趋及其生态毒性研究进展[J].生态学杂志,31(12):3228-3234
郭丽.2015.环丙沙星在潮土中吸附-解吸特性及运移规律研究[D].北京:中国科学院大学
Hernando M D,Mezcua M,Fernandezalba A R,et al.2006.Environmental risk assessment of pharmaceutical residues in wastewater effluents,surface waters and sediments[J].Talanta,69(2):334-342
Ho Y B,Zakaria M P,Latif P A,et al.2014.Occurrence of veterinary antibiotics and progesterone in broiler manure and agricultural soil in Malaysia[J].Science of the Total Environment,488-489(1):261-267
Huang Y J,Cheng M M,Li W H,et al.2013.Simultaneous extraction of four classes of antibiotics in soil,manure and sewage sludge and analysis by liquid chromatography-tandem mass spectrometry with the isotope-labelled internal standard method[J].Analytical Methods,5:3721-3731
Jjemba P K.2002.The potential impact of veterinary and human therapeutic agents in manure and biosolids on plants grown on arable land:a review[J].Agriculture,Ecosystems & Environment,93:267-278
Lapworth D J,Baran N,Stuart M E,et al.2012.Emerging organic contaminants in groundwater:a review of sources,fate and occurrence[J].Environmental Pollution,163:287-303
Leal R M P,Luis Reynaldo Ferracciú Alleoni,Tornisielo V L,et al.2013.Sorption of fluoroquinolones and sulfonamides in 13 Brazilian soils[J].Chemosphere,92(8):979-985
Leeuwen K V.1996.Technical guidance document in support of Commission directive 93/67 EEC on risk assessment for new notified substances and Commission regulation (EC) No.1488/94 on risk assessment for existing substances[M].Office for Official Public of the European Communities
Li B,Zhang T,Xu Z,et al.2009.Rapid analysis of 21 antibiotics of multiple classes in municipal wastewater using ultra performance liquid chromatography-tandem mass spectrometry[J].Analytica Chimica Acta,645(1):64-72
Li N,Zhang X,Wu W,et al.2014.Occurrence,seasonal variation and risk assessment of antibiotics in the reservoirs in North China[J].Chemosphere,111:327-335
李学菊.2012.抗生素滥用后果分析[J].临床合理用药杂志,5(11):130-130
Li Y W,Wu X L,Mo C H,et al.2011.Investigation of sulfonamide,tetracycline,and quinolone antibiotics in vegetable farmland soil in the Pearl River Delta area,southern China[J].Journal of Agricultural and Food Chemistry,59(13):7268-7276
刘锋,廖德润,李可,等.2013.畜禽养殖基地磺胺类喹诺酮类和大环内酯类抗生素污染特征[J].农业环境科学学报,32(4):847-853
Liu F,Ying G G,Tao R,et al.2009.Effects of six selected antibiotics on plant growth and soil microbial and enzymatic activities[J].Environmental Pollution,157:1636-1642
刘明亮.2006.喹诺酮类抗菌药在不同介质中的理化性质[J].国外医药(抗生素分册),27(1),22-34
Liu X,Lu S,Guo W,et al.2018.Antibiotics in the aquatic environments:A review of lakes,China[J].Science of the Total Environment,627:1195-1208
Liu X,Steele J C,Meng X Z.2017.Usage,residue,and human health risk of antibiotics in Chinese aquaculture:A review[J].Environmental Pollution,223:161-169
MartínezCarballo E,GonzálezBarreiro C,Scharf S,et al.2007.Environmental monitoring study of selected veterinary antibiotics in animal manure and soils in Austria[J].Environmental Pollution,148(2):570-579
Pan M,Chu L M.2017.Fate of antibiotics in soil and their uptake by edible crops[J].Science of the Total Environment,s 599-600:500-512
Pan M,Chu L M.2016.Adsorption and degradation of five selected antibiotics in agricultural soil[J].Science of The Total Environment,545-546:48-56
Park H R,Kim T H,Bark K M.2002.Physicochemical properties of quinolone antibiotics in various environments[J].European Journal of Medicinal Chemistry,37(6):443-460
齐会勉,吕亮,乔显亮.2009.抗生素在土壤中的吸附行为研究进展[J].土壤,41(5):703-708
Sassman S A,Lee L S.2005.Sorption of three tetracyclines by several soils:assessing the role of pH and cation exchange[J].Environmental Science & Technology,39(19):7452-7459
史烨弘.2004.沉积物和腐殖质对几种多环芳烃的吸附特征研究[D].北京:北京师范大学
苏思慧,何江涛,杨蕾,等.2014.北京东南郊土壤剖面氟喹诺酮类抗生素分布特征[J].环境科学,11:4257-4266
王敏,唐景春.2010.土壤中的抗生素污染及其生态毒性研究进展[J].农业环境科学学报,29(S1):261-266
王朋.2013.氧氟沙星在不同性质吸附剂上的吸附动力学研究[D].昆明:昆明理工大学
Wang S,Wang H.2015.Adsorption behavior of antibiotic in soil environment:a critical review[J].Frontiers of Environmental Science & Engineering,9(4):565-574
汪小兰.2005.有机化学-第4版[M].北京:高等教育出版社
Wu X,Wei Y,Zheng J,et al.2011.The behavior of tetracyclines and their degradation products during swine manure composting[J].Bioresource Technology,102(10):5924-5931
Wu X L,Xiang L,Yan Q Y,et al.2014.Distribution and risk assessment of quinolone antibiotics in the soils from organic vegetable farms of a subtropical city,Southern China.[J].Science of the Total Environment,487(1):399-406
Yang Y,Owino A A,Gao Y,et al.2016.Occurrence,composition and risk assessment of antibiotics in soils from Kenya,Africa[J].Ecotoxicology,25(6):1194-1201
伊丽丽.2013.再生水灌溉典型药物土壤环境行为与生态风险研究[D].北京:中国科学院大学
尹春艳,骆永明,滕应,等.2012.典型设施菜地土壤抗生素污染特征与积累规律研究[J].环境科学,33(8):2810-2816
Zhang J,Li Z J,Ge G F,et al.2009.Impacts of soil organic matter,pH and exogenous copper on sorption behavior of norfloxacin in three soils[J].Journal of Environmental Science,21:632-640
张劲强,董元华.2007.诺氟沙星在4种土壤中的吸附-解吸特征[J].环境科学,28(9):2134-2140
张娟.2011.磺胺嘧啶与铜在土壤中的吸附行为及其影响因素的研究[D].镇江:江苏科技大学
张侃侃,郭文炯.2017.汾河流域城镇化进程及影响因素分析[J].中国名城,10:20-27
Zhang Q Q,Ying G G,Pan C G,et al.2015.Comprehensive evaluation of antibiotics emission and fate in the river basins of china:source analysis,multimedia modeling,and linkage to bacterial resistance[J].Environmental Science & Technology,49(11):6772-6782
张涛,郭晓,刘俊杰,等.2017.江西梅江流域土壤中四环素类抗生素的含量及空间分布特征[J].环境科学学报,37(4):1493-1501
Zhao J L,Ying G G,Liu Y S,et al.2010.Occurrence and a screening-level risk assessment of human pharmaceuticals in the Pearl River system,South China[J].Environmental Toxicology & Chemistry,29(6):1377-1384
Borecka M,Anna B B,Siedlewicz G,et al.2013.A new approach for the estimation of expanded uncertainty of results of an analytical method developed for determining antibiotics in seawater using solid-phase extraction disks and liquid chromatography coupled with tandem mass spectrometry technique[J].Journal of Chromatography A,1304:138-146
Briones R M,Sarmah A K,Padhye L P.2016.A global perspective on the use,occurrence,fate and effects of anti-diabetic drug metformin in natural and engineered ecosystems[J].Environmental Pollution,219:1007-1020
Bruchet A,Hochereau C,Picard C,et al.2005.Analysis of drugs and personal care products in French source and drinking waters:the analytical challenge and examples of application[J].Water Science& Technology,52(8):53-61
陈昦,董元华,王辉,等.2008.江苏省畜禽粪便中磺胺类药物残留特征[J].农业环境科学学报,27(1):385-389
Conkle J L,Lattao C,White J R,et al.2010.Competitive sorption and desorption behavior for three fluoroquinolone antibiotics in a wastewater treatment wetland soil[J].Chemosphere,80(11):1353-1359
Doorslaer X V,Dewulf J,Langenhove H V,et al.2014.Fluoroquinolone antibiotics:An emerging class of environmental micropollutants[J].Science of the Total Environment,500-501(1/3):250-269
Dorival-García,N,Zafra-Gómez,A,Navalón,A,et al.2013.Removal of quinolone antibiotics from wastewaters by sorption and biological degradation in laboratory-scale membrane bioreactors[J].Science of The Total Environment,442(Complete):317-328
Ebert I,Bachmann J,Kühnen U,et al.2011.Toxicity of the fluoroquinolone antibiotics enrofloxacin and ciprofloxacin to photoautotrophic aquatic organisms[J].Environmental Toxicology and Chemistry,30(12):2786-2792
方旭婷,任珂君,刘玉,等.2016.广东一饮用水源地河流沉积物及鱼体中氟喹诺酮类(FQs)抗生素残留特征研究[J].环境科学学报,36(3):760-766
冯佳,郭宇宁,王飞,等.2016.太原汾河景区浮游植物群落结构及其与环境因子关系分析[J].环境科学,37(4):1353-1361
Gong W,Liu X,He H,et al.2012.Quantitatively modeling soil-water distribution coefficients of three antibiotics using soil physicochemical properties[J].Chemosphere,89(7):825-831
Grenni P,Ancona V,Barra A.2017.Ecological effects of antibiotics on natural ecosystems:A review[J].Microchemical Journal,136:25-39
管荷兰,于海凤,王嘉宇.2012.氟喹诺酮类抗生素在土壤中的归趋及其生态毒性研究进展[J].生态学杂志,31(12):3228-3234
郭丽.2015.环丙沙星在潮土中吸附-解吸特性及运移规律研究[D].北京:中国科学院大学
Hernando M D,Mezcua M,Fernandezalba A R,et al.2006.Environmental risk assessment of pharmaceutical residues in wastewater effluents,surface waters and sediments[J].Talanta,69(2):334-342
Ho Y B,Zakaria M P,Latif P A,et al.2014.Occurrence of veterinary antibiotics and progesterone in broiler manure and agricultural soil in Malaysia[J].Science of the Total Environment,488-489(1):261-267
Huang Y J,Cheng M M,Li W H,et al.2013.Simultaneous extraction of four classes of antibiotics in soil,manure and sewage sludge and analysis by liquid chromatography-tandem mass spectrometry with the isotope-labelled internal standard method[J].Analytical Methods,5:3721-3731
Jjemba P K.2002.The potential impact of veterinary and human therapeutic agents in manure and biosolids on plants grown on arable land:a review[J].Agriculture,Ecosystems & Environment,93:267-278
Lapworth D J,Baran N,Stuart M E,et al.2012.Emerging organic contaminants in groundwater:a review of sources,fate and occurrence[J].Environmental Pollution,163:287-303
Leal R M P,Luis Reynaldo Ferracciú Alleoni,Tornisielo V L,et al.2013.Sorption of fluoroquinolones and sulfonamides in 13 Brazilian soils[J].Chemosphere,92(8):979-985
Leeuwen K V.1996.Technical guidance document in support of Commission directive 93/67 EEC on risk assessment for new notified substances and Commission regulation (EC) No.1488/94 on risk assessment for existing substances[M].Office for Official Public of the European Communities
Li B,Zhang T,Xu Z,et al.2009.Rapid analysis of 21 antibiotics of multiple classes in municipal wastewater using ultra performance liquid chromatography-tandem mass spectrometry[J].Analytica Chimica Acta,645(1):64-72
Li N,Zhang X,Wu W,et al.2014.Occurrence,seasonal variation and risk assessment of antibiotics in the reservoirs in North China[J].Chemosphere,111:327-335
李学菊.2012.抗生素滥用后果分析[J].临床合理用药杂志,5(11):130-130
Li Y W,Wu X L,Mo C H,et al.2011.Investigation of sulfonamide,tetracycline,and quinolone antibiotics in vegetable farmland soil in the Pearl River Delta area,southern China[J].Journal of Agricultural and Food Chemistry,59(13):7268-7276
刘锋,廖德润,李可,等.2013.畜禽养殖基地磺胺类喹诺酮类和大环内酯类抗生素污染特征[J].农业环境科学学报,32(4):847-853
Liu F,Ying G G,Tao R,et al.2009.Effects of six selected antibiotics on plant growth and soil microbial and enzymatic activities[J].Environmental Pollution,157:1636-1642
刘明亮.2006.喹诺酮类抗菌药在不同介质中的理化性质[J].国外医药(抗生素分册),27(1),22-34
Liu X,Lu S,Guo W,et al.2018.Antibiotics in the aquatic environments:A review of lakes,China[J].Science of the Total Environment,627:1195-1208
Liu X,Steele J C,Meng X Z.2017.Usage,residue,and human health risk of antibiotics in Chinese aquaculture:A review[J].Environmental Pollution,223:161-169
MartínezCarballo E,GonzálezBarreiro C,Scharf S,et al.2007.Environmental monitoring study of selected veterinary antibiotics in animal manure and soils in Austria[J].Environmental Pollution,148(2):570-579
Pan M,Chu L M.2017.Fate of antibiotics in soil and their uptake by edible crops[J].Science of the Total Environment,s 599-600:500-512
Pan M,Chu L M.2016.Adsorption and degradation of five selected antibiotics in agricultural soil[J].Science of The Total Environment,545-546:48-56
Park H R,Kim T H,Bark K M.2002.Physicochemical properties of quinolone antibiotics in various environments[J].European Journal of Medicinal Chemistry,37(6):443-460
齐会勉,吕亮,乔显亮.2009.抗生素在土壤中的吸附行为研究进展[J].土壤,41(5):703-708
Sassman S A,Lee L S.2005.Sorption of three tetracyclines by several soils:assessing the role of pH and cation exchange[J].Environmental Science & Technology,39(19):7452-7459
史烨弘.2004.沉积物和腐殖质对几种多环芳烃的吸附特征研究[D].北京:北京师范大学
苏思慧,何江涛,杨蕾,等.2014.北京东南郊土壤剖面氟喹诺酮类抗生素分布特征[J].环境科学,11:4257-4266
王敏,唐景春.2010.土壤中的抗生素污染及其生态毒性研究进展[J].农业环境科学学报,29(S1):261-266
王朋.2013.氧氟沙星在不同性质吸附剂上的吸附动力学研究[D].昆明:昆明理工大学
Wang S,Wang H.2015.Adsorption behavior of antibiotic in soil environment:a critical review[J].Frontiers of Environmental Science & Engineering,9(4):565-574
汪小兰.2005.有机化学-第4版[M].北京:高等教育出版社
Wu X,Wei Y,Zheng J,et al.2011.The behavior of tetracyclines and their degradation products during swine manure composting[J].Bioresource Technology,102(10):5924-5931
Wu X L,Xiang L,Yan Q Y,et al.2014.Distribution and risk assessment of quinolone antibiotics in the soils from organic vegetable farms of a subtropical city,Southern China.[J].Science of the Total Environment,487(1):399-406
Yang Y,Owino A A,Gao Y,et al.2016.Occurrence,composition and risk assessment of antibiotics in soils from Kenya,Africa[J].Ecotoxicology,25(6):1194-1201
伊丽丽.2013.再生水灌溉典型药物土壤环境行为与生态风险研究[D].北京:中国科学院大学
尹春艳,骆永明,滕应,等.2012.典型设施菜地土壤抗生素污染特征与积累规律研究[J].环境科学,33(8):2810-2816
Zhang J,Li Z J,Ge G F,et al.2009.Impacts of soil organic matter,pH and exogenous copper on sorption behavior of norfloxacin in three soils[J].Journal of Environmental Science,21:632-640
张劲强,董元华.2007.诺氟沙星在4种土壤中的吸附-解吸特征[J].环境科学,28(9):2134-2140
张娟.2011.磺胺嘧啶与铜在土壤中的吸附行为及其影响因素的研究[D].镇江:江苏科技大学
张侃侃,郭文炯.2017.汾河流域城镇化进程及影响因素分析[J].中国名城,10:20-27
Zhang Q Q,Ying G G,Pan C G,et al.2015.Comprehensive evaluation of antibiotics emission and fate in the river basins of china:source analysis,multimedia modeling,and linkage to bacterial resistance[J].Environmental Science & Technology,49(11):6772-6782
张涛,郭晓,刘俊杰,等.2017.江西梅江流域土壤中四环素类抗生素的含量及空间分布特征[J].环境科学学报,37(4):1493-1501
Zhao J L,Ying G G,Liu Y S,et al.2010.Occurrence and a screening-level risk assessment of human pharmaceuticals in the Pearl River system,South China[J].Environmental Toxicology & Chemistry,29(6):1377-1384
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