广西会仙岩溶湿地典型抗生素污染特征及生态风险评估
|
摘要
为确定会仙岩溶湿地不同介质中抗生素的污染特征及来源,利用液相色谱串联质谱联用仪分析了磺胺类(SAs)、氟喹诺酮类(FQs)和四环素类(TCs)三大类20种抗生素的含量.结果表明,研究区内水土介质监测的抗生素中共检出12种,检出浓度范围为n.d～106 ng·L~(-1),其中,甲氧苄氨嘧啶(TMP)的浓度最高.各环境介质中,以养殖用水和地表河水中检出的抗生素种类相对较多,分别为10种和8种,溶潭水和土壤中则检出的抗生素种类较少.因子分析结果显示,会仙湿地水体中的典型抗生素来源可归为两类,一类以受外源污染为主,从而导致地表河水中磺胺氯达嗪(SCP)、磺胺嘧啶(SDZ)、磺胺甲恶唑(SMZ)、诺氟沙星(NOR)、氧氟沙星(OFL)检出浓度较高,一类受湿地内养殖污染,从而造成水土介质中磺胺二甲基嘧啶(SMD)、甲氧苄氨嘧啶(TMP)和金霉素(CTC)检出.水体中检出的抗生素主要受溶解氧(DO)影响,此外,甲氧苄氨嘧啶(TMP)、恩诺沙星(ENR)和强力霉素(DOX)与NH~+_4存在一定的协同污染关系.风险评估结果表明,恩诺沙星(ENR)处于高风险的范围内,磺胺甲恶唑(SMZ)、诺氟沙星(NOR)和氧氟沙星(OFL)处于中等风险,中等风险的抗生素主要集中在地表河水中,高风险抗生素则在养殖用水中.整体来看,研究区水体中抗生素存在一定的风险.因此,针对这一现象应减少存在生态风险抗生素的使用,并对有潜在风险的抗生素加以防范.
In order to determine the pollution characteristics and sources of antibiotics in different media of Huixian Karst wetland, the liquid chromatography tandem mass spectrometry(LC-MS/MS) was used to analyze the contents of sulfonamides(SAs), fluoroquinolones(FQs), tetracyclines(TCs). The results showed that 12 of the 20 antibiotics were detected in the water and soil of the study area. The mass concentrations of the 12 antibiotics ranged from N.D to 106 ng·L~(-1), among which the concentration of trimethoprim(TMP) was the highest. There were 10 and 8 kinds of antibiotics were detected in aquaculture water and surface water respectively, while less kinds of antibiotics were detected in solution pool water and soil. The factor analysis showed that the typical antibiotics in Huixian wetland water can be classified into two categories. One was the detection concentration of sulfachlordazine(SCP), sulfadiazine(SDZ), sulfamethoxazole(SMZ), norfloxacin(NOR) and ofloxacin(OFL) in surface river water caused mainly by exogenous pollution. The other one was the detection of sulfamethazine(SMD), trimethoprim(TMP) and chlortetracycline(CTC) in soil and water caused by aquaculturepollution in wetland. The antibiotics detected in water were mainly affected by dissolved oxygen(DO). In addition, there was a synergistic pollution relationship between trimethoprim(TMP), enrofloxacin(ENR), doxycycline(DOX) and NH~+_4. The results of risk assessment showed that the enrofloxacin(ENR) was at high risk, while the sulfamethoxazole(SMZ), norfloxacin(NOR) and ofloxacin(OFL) were at moderate risk. The moderate-risk antibiotics were mainly concentrated in the surface river water, while the high-risk antibiotics were in the aquaculture water. Overall, there was a certain risk of antibiotics in the waters of the study area. Therefore, the use reduction of antibiotics with ecological risks and the precautions against antibiotics with potential risks should be taken into consideration.
In order to determine the pollution characteristics and sources of antibiotics in different media of Huixian Karst wetland, the liquid chromatography tandem mass spectrometry(LC-MS/MS) was used to analyze the contents of sulfonamides(SAs), fluoroquinolones(FQs), tetracyclines(TCs). The results showed that 12 of the 20 antibiotics were detected in the water and soil of the study area. The mass concentrations of the 12 antibiotics ranged from N.D to 106 ng·L~(-1), among which the concentration of trimethoprim(TMP) was the highest. There were 10 and 8 kinds of antibiotics were detected in aquaculture water and surface water respectively, while less kinds of antibiotics were detected in solution pool water and soil. The factor analysis showed that the typical antibiotics in Huixian wetland water can be classified into two categories. One was the detection concentration of sulfachlordazine(SCP), sulfadiazine(SDZ), sulfamethoxazole(SMZ), norfloxacin(NOR) and ofloxacin(OFL) in surface river water caused mainly by exogenous pollution. The other one was the detection of sulfamethazine(SMD), trimethoprim(TMP) and chlortetracycline(CTC) in soil and water caused by aquaculturepollution in wetland. The antibiotics detected in water were mainly affected by dissolved oxygen(DO). In addition, there was a synergistic pollution relationship between trimethoprim(TMP), enrofloxacin(ENR), doxycycline(DOX) and NH~+_4. The results of risk assessment showed that the enrofloxacin(ENR) was at high risk, while the sulfamethoxazole(SMZ), norfloxacin(NOR) and ofloxacin(OFL) were at moderate risk. The moderate-risk antibiotics were mainly concentrated in the surface river water, while the high-risk antibiotics were in the aquaculture water. Overall, there was a certain risk of antibiotics in the waters of the study area. Therefore, the use reduction of antibiotics with ecological risks and the precautions against antibiotics with potential risks should be taken into consideration.
引文
Alam M J,Yuan D X,Jiang Y J,et al.2014.Sources and transports of polycyclic aromatic hydrocarbons in the Nanshan Underground River China[J].Environment Earth Science,71(4):1967-1976
Balakrishna K,Rath A,Praveenkumarreddy Y,et al.2016.A review of the occurrence of pharmaceuticals and personal care products in Indian water bodies[J].Ecotoxicology & Environmental Safety,137:113
Biak-Bielińska A,Stolte S,Arning J,et al.2011.Ecotoxicity evaluation of selected sulfonamides[J].Chemosphere,85(6):928-933
Bona M D,Di Leva V,De Liguoro M.2014.The sensitivity of Daphnia magna and Daphnia curvirostris to 10 veterinary antibacterials and to some of their binary mixtures[J].Chemosphere,115:67-74
Cheng D,Liu X,Wang L,et al.2014.Seasonal variation and sediment-water exchange of antibiotics in a shallower large lake in North China[J].Science of the Total Environment,476-477:266-275
Chiffre A,Degiorgi F,Bulete A,et al.2016.Occurrence of pharmaceuticals in WWTP effluents and their impact in a karstic rural catchment of eastern France[J].Environmental Science Processes & Research,23:25427-25441
蔡德所,马祖陆,赵湘桂,等.2009.桂林会仙岩溶湿地近40年演变的遥感监测[J].广西师范大学学报(自然科学版),27(2):111-117
Dantas G,Sommer M O,Oluwasegun R D,et al.2008.Bacteria subsisting on antibiotics[J].Science,320(5872):100-103
Daughton C G,Ternes T A.1999.Pharmaceuticals and personal care products in the environment:agents of subtle change?[J].Environmental Health Perspectives,107(suppl 6):907-938
Dodgen L K,Kelly W R,Panno S V,et al.2017.Characterizing pharmaceutical,personal care product,and hormone contamination in a karst aquifer of southwestern Illinois,USA,using water quality and stream flow parameters[J].Science of the Total Environment,578:281-289
邓旺明,李浩瑜,刘士涛,等.2016.水产养殖业抗生素在水环境中的迁移转化[J].广东化工,43(3):91-92
European Commission.2003.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 Substance[M].Luxembourg:Office for Official Publications of the European Communities
Garcíagalán M J,Garrido T,Fraile J,et al.2010.Simultaneous occurrence of nitrates and sulfonamide antibiotics in two ground water bodies of Catalonia (Spain)[J].Journal of Hydrology,383(1):93-101
Hernando M D,Mezcua M,Fernández-Alba A R,et al.2006.Environmental risk assessment of pharmaceutical residues in wastewater effluents,surface waters and sediments[J].Talanta,69(2):334-342
Hillebrand O,Noedler K,Sauter M,et al.2015.Multitracer experiment to evaluate the attenuation of selected organic micropollutants in a karst aquifer[J].Science of the Total Environment,506:338-343
Hu X,Zhou Q,Luo Y.2010.Occurrence and source analysis of typical veterinary antibiotics in manure,soil,vegetables and groundwater from organic vegetable bases,northern China[J].Environmental Pollution,158(9):2992-2998
Huang F Y,Zou S Z,Deng D D,et al.2019.Antibiotics in a typical karst river system in China:Spatiotemporal variation and environmental risks[J].Science of the Total Environment,650:1348-1355
Isidori M,Lavorgna M,Nardelli A,et al.2005.Toxic and genotoxic evaluation of six antibiotics on non-target organisms[J].Science of the Total Environment,346(1/3):87-98
靳振江,程亚平,李强,等.2014.会仙喀斯特溶洞湿地、稻田和旱田土壤有机碳含量及其与养分的关系[J].湿地科学,12(4):485-490
Liang X,Chen B,Nie X,et al.2013.The distribution and partitioning of common antibiotics in water and sediment of the Pearl River Estuary,South China[J].Chemosphere,92(11):1410-1416
Lin A Y,Yu T H,Lin C F.2008.Pharmaceutical contamination in residential,industrial and agricultural waste streams:risk to aqueous environments in Taiwan[J].Chemosphere,74(1):131-141
Martinez J L.2008.Antibiotics and antibiotic resistance genes in natural environments[J].Science,321(5887):365-367
Pan M,Chu L M.2018.Occurrence of antibiotics and antibiotic resistance genes in soils from wastewater irrigation areas in the Pearl River Delta region,southern China[J].Science of the Total Environment,624:145-152
彭聪,潘晓东,焦友军,等.2018.多种同位素手段的硝酸盐污染源解析:以会仙湿地为例[J].环境科学,39(12):5410-5417
全瑶,毕二平.2017.不同形态的氧氟沙星在凹凸棒土上的吸附特征[J].高等学校化学学报,38(4):622-630
Riaz L,Mahmood T,Khalid A,et al.2018.Fluoroquinolones (FQs) in the environment:a review on their abundance,sorption and toxicity in soil[J].Chemosphere,191:704-720
Shi H,Yang Y,Liu M,et al.2014.Occurrence and distribution of antibiotics in the surface sediments of the Yangtze Estuary and nearby coastal areas[J].Marine Pollution Bulletin,83(1):317-323
Simazaki D,Kubota R,Suzuki T,et al.2015.Occurrence of selected pharmaceuticals at drinking water purification plants in Japan and implications for human health[J].Water Research,76:187-200
Stuer-Lauridsen F,Birkved M,Hansen L P,et al.2000.Environmental risk assessment of human pharmaceuticals in Denmark after normal therapeutic use[J].Chemosphere,40(7):783-793
Szekeres E,Chiriac C M,Baricz A,et al.2018.Investigating antibiotics,antibiotic resistance genes,and microbial contaminants in groundwater in relation to the proximity of urban areas[J].Environmental Pollution,236:734-744
孙凯.2015.洪泽湖湿地典型抗生素污染特征与生态风险[D].南京:南京林业大学
Tang J,Shi T,Wu X,et al.2015.The occurrence and distribution of antibiotics in Lake Chaohu,China:Seasonal variation,potential source and risk assessment[J].Chemosphere,122:154-161
Tong L,Qin L,Xie C,et al.2017.Distribution of antibiotics in alluvial sediment near animal breeding areas at the Jianghan Plain,Central China[J].Chemosphere,186:100-107
Turkdogan F I,Yetilmezsoy K.2009.Appraisal of potential environmental risks associated with human antibiotic consumption in Turkey[J].Journal of Hazardous Materials,166(1):297-308
童蕾,姚林林,刘慧,等.2016.抗生素在地下水系统中的环境行为及生态效应研究进展[J].生态毒理学报,11(2):27-36
Vryzas Z,Alexoudis C,Vassiliou G,et al.2011.Determination and aquatic risk assessment of pesticide residues in riparian drainage canals in northeastern Greece[J].Ecotoxicology and Environmental Safety,74(2):174-181
World Health Organization.2014.Antimicrobial Resistance:Global Report on Surveillance[M].Geneva:World Health Organization
王冉,刘铁铮,王恬.2006 抗生素在环境中的转归及其生态毒性[J].生态学报,26(1):265-270
尉小旋,陈景文,王如冰,等.2015.氧氟沙星和诺氟沙星的水环境光化学转化:pH 值及溶解性物质的影响[J].环境化学,34(3):448-454
Xu W,Zhang G,Li X,et al.2007.Occurrence and elimination of antibiotics at four sewage treatment plants in the Pearl River Delta (PRD),South China[J].Water Research,41(19):4526-4534
Xue B M,Zhang R J,Wang Y H,et al.2013.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[J].Ecotoxicology and Environmental Safety,92:229-236
Yan C,Yang Y,Zhou J,et al.2013.Antibiotics in the surface water of the Yangtze Estuary:occurrence,distribution and risk assessment[J].Environmental Pollution,175(8):22-29
叶为民,黄伟,陈宝,郁陈,王驹.2009.双电层理论与高庙子膨润土的体变特征[J].岩土力学,30(7):1899-1903
Zhang M W,Jin H J,Cai D S,et al.2010.The comparative study on the ecological sensitivity analysis in Huixian Karst Wetland,China[J].Procedia Environmental Sciences,2(1):386-398
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,49:6772-6782
周爱霞.2015.潜水中磺胺抗生素迁移转化机理及修复技术研究[D].长春:吉林大学
Zhou L J,Ying G G,Zhao J L,et al.2011.Trends in the occurrence of human and veterinary antibiotics in the sediments of the Yellow River,Hai River and Liao River in northern China[J].Environmental Pollution,159(7):1877-1885
Zou S Z,Huang F Y,Chen L,et al.2018.The occurrence and distribution of antibiotics in the Karst River system in Kaiyang,Southwest China[J].Water Science Technology:Water Supply.18(6):2044-2052
Balakrishna K,Rath A,Praveenkumarreddy Y,et al.2016.A review of the occurrence of pharmaceuticals and personal care products in Indian water bodies[J].Ecotoxicology & Environmental Safety,137:113
Biak-Bielińska A,Stolte S,Arning J,et al.2011.Ecotoxicity evaluation of selected sulfonamides[J].Chemosphere,85(6):928-933
Bona M D,Di Leva V,De Liguoro M.2014.The sensitivity of Daphnia magna and Daphnia curvirostris to 10 veterinary antibacterials and to some of their binary mixtures[J].Chemosphere,115:67-74
Cheng D,Liu X,Wang L,et al.2014.Seasonal variation and sediment-water exchange of antibiotics in a shallower large lake in North China[J].Science of the Total Environment,476-477:266-275
Chiffre A,Degiorgi F,Bulete A,et al.2016.Occurrence of pharmaceuticals in WWTP effluents and their impact in a karstic rural catchment of eastern France[J].Environmental Science Processes & Research,23:25427-25441
蔡德所,马祖陆,赵湘桂,等.2009.桂林会仙岩溶湿地近40年演变的遥感监测[J].广西师范大学学报(自然科学版),27(2):111-117
Dantas G,Sommer M O,Oluwasegun R D,et al.2008.Bacteria subsisting on antibiotics[J].Science,320(5872):100-103
Daughton C G,Ternes T A.1999.Pharmaceuticals and personal care products in the environment:agents of subtle change?[J].Environmental Health Perspectives,107(suppl 6):907-938
Dodgen L K,Kelly W R,Panno S V,et al.2017.Characterizing pharmaceutical,personal care product,and hormone contamination in a karst aquifer of southwestern Illinois,USA,using water quality and stream flow parameters[J].Science of the Total Environment,578:281-289
邓旺明,李浩瑜,刘士涛,等.2016.水产养殖业抗生素在水环境中的迁移转化[J].广东化工,43(3):91-92
European Commission.2003.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 Substance[M].Luxembourg:Office for Official Publications of the European Communities
Garcíagalán M J,Garrido T,Fraile J,et al.2010.Simultaneous occurrence of nitrates and sulfonamide antibiotics in two ground water bodies of Catalonia (Spain)[J].Journal of Hydrology,383(1):93-101
Hernando M D,Mezcua M,Fernández-Alba A R,et al.2006.Environmental risk assessment of pharmaceutical residues in wastewater effluents,surface waters and sediments[J].Talanta,69(2):334-342
Hillebrand O,Noedler K,Sauter M,et al.2015.Multitracer experiment to evaluate the attenuation of selected organic micropollutants in a karst aquifer[J].Science of the Total Environment,506:338-343
Hu X,Zhou Q,Luo Y.2010.Occurrence and source analysis of typical veterinary antibiotics in manure,soil,vegetables and groundwater from organic vegetable bases,northern China[J].Environmental Pollution,158(9):2992-2998
Huang F Y,Zou S Z,Deng D D,et al.2019.Antibiotics in a typical karst river system in China:Spatiotemporal variation and environmental risks[J].Science of the Total Environment,650:1348-1355
Isidori M,Lavorgna M,Nardelli A,et al.2005.Toxic and genotoxic evaluation of six antibiotics on non-target organisms[J].Science of the Total Environment,346(1/3):87-98
靳振江,程亚平,李强,等.2014.会仙喀斯特溶洞湿地、稻田和旱田土壤有机碳含量及其与养分的关系[J].湿地科学,12(4):485-490
Liang X,Chen B,Nie X,et al.2013.The distribution and partitioning of common antibiotics in water and sediment of the Pearl River Estuary,South China[J].Chemosphere,92(11):1410-1416
Lin A Y,Yu T H,Lin C F.2008.Pharmaceutical contamination in residential,industrial and agricultural waste streams:risk to aqueous environments in Taiwan[J].Chemosphere,74(1):131-141
Martinez J L.2008.Antibiotics and antibiotic resistance genes in natural environments[J].Science,321(5887):365-367
Pan M,Chu L M.2018.Occurrence of antibiotics and antibiotic resistance genes in soils from wastewater irrigation areas in the Pearl River Delta region,southern China[J].Science of the Total Environment,624:145-152
彭聪,潘晓东,焦友军,等.2018.多种同位素手段的硝酸盐污染源解析:以会仙湿地为例[J].环境科学,39(12):5410-5417
全瑶,毕二平.2017.不同形态的氧氟沙星在凹凸棒土上的吸附特征[J].高等学校化学学报,38(4):622-630
Riaz L,Mahmood T,Khalid A,et al.2018.Fluoroquinolones (FQs) in the environment:a review on their abundance,sorption and toxicity in soil[J].Chemosphere,191:704-720
Shi H,Yang Y,Liu M,et al.2014.Occurrence and distribution of antibiotics in the surface sediments of the Yangtze Estuary and nearby coastal areas[J].Marine Pollution Bulletin,83(1):317-323
Simazaki D,Kubota R,Suzuki T,et al.2015.Occurrence of selected pharmaceuticals at drinking water purification plants in Japan and implications for human health[J].Water Research,76:187-200
Stuer-Lauridsen F,Birkved M,Hansen L P,et al.2000.Environmental risk assessment of human pharmaceuticals in Denmark after normal therapeutic use[J].Chemosphere,40(7):783-793
Szekeres E,Chiriac C M,Baricz A,et al.2018.Investigating antibiotics,antibiotic resistance genes,and microbial contaminants in groundwater in relation to the proximity of urban areas[J].Environmental Pollution,236:734-744
孙凯.2015.洪泽湖湿地典型抗生素污染特征与生态风险[D].南京:南京林业大学
Tang J,Shi T,Wu X,et al.2015.The occurrence and distribution of antibiotics in Lake Chaohu,China:Seasonal variation,potential source and risk assessment[J].Chemosphere,122:154-161
Tong L,Qin L,Xie C,et al.2017.Distribution of antibiotics in alluvial sediment near animal breeding areas at the Jianghan Plain,Central China[J].Chemosphere,186:100-107
Turkdogan F I,Yetilmezsoy K.2009.Appraisal of potential environmental risks associated with human antibiotic consumption in Turkey[J].Journal of Hazardous Materials,166(1):297-308
童蕾,姚林林,刘慧,等.2016.抗生素在地下水系统中的环境行为及生态效应研究进展[J].生态毒理学报,11(2):27-36
Vryzas Z,Alexoudis C,Vassiliou G,et al.2011.Determination and aquatic risk assessment of pesticide residues in riparian drainage canals in northeastern Greece[J].Ecotoxicology and Environmental Safety,74(2):174-181
World Health Organization.2014.Antimicrobial Resistance:Global Report on Surveillance[M].Geneva:World Health Organization
王冉,刘铁铮,王恬.2006 抗生素在环境中的转归及其生态毒性[J].生态学报,26(1):265-270
尉小旋,陈景文,王如冰,等.2015.氧氟沙星和诺氟沙星的水环境光化学转化:pH 值及溶解性物质的影响[J].环境化学,34(3):448-454
Xu W,Zhang G,Li X,et al.2007.Occurrence and elimination of antibiotics at four sewage treatment plants in the Pearl River Delta (PRD),South China[J].Water Research,41(19):4526-4534
Xue B M,Zhang R J,Wang Y H,et al.2013.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[J].Ecotoxicology and Environmental Safety,92:229-236
Yan C,Yang Y,Zhou J,et al.2013.Antibiotics in the surface water of the Yangtze Estuary:occurrence,distribution and risk assessment[J].Environmental Pollution,175(8):22-29
叶为民,黄伟,陈宝,郁陈,王驹.2009.双电层理论与高庙子膨润土的体变特征[J].岩土力学,30(7):1899-1903
Zhang M W,Jin H J,Cai D S,et al.2010.The comparative study on the ecological sensitivity analysis in Huixian Karst Wetland,China[J].Procedia Environmental Sciences,2(1):386-398
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,49:6772-6782
周爱霞.2015.潜水中磺胺抗生素迁移转化机理及修复技术研究[D].长春:吉林大学
Zhou L J,Ying G G,Zhao J L,et al.2011.Trends in the occurrence of human and veterinary antibiotics in the sediments of the Yellow River,Hai River and Liao River in northern China[J].Environmental Pollution,159(7):1877-1885
Zou S Z,Huang F Y,Chen L,et al.2018.The occurrence and distribution of antibiotics in the Karst River system in Kaiyang,Southwest China[J].Water Science Technology:Water Supply.18(6):2044-2052