2种经典模型对抗生素与重金属锌的蛋白核小球藻时间依赖联合毒性作用的评估比较
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摘要
污染物在环境中普遍以混合物的形式存在,其累积毒性与毒性相互作用具有潜在的环境风险。因此,本研究以水环境中普遍存在的氨基糖苷类抗生素(硫酸链霉素、硫酸安普霉素和双氢链霉素)和重金属锌(Zn)为目标污染物,以蛋白核小球藻(Chlorella pyrenoidosa,C. pyrenoidosa)为指示生物,应用直接均分射线法设计3种抗生素与Zn的3个二元混合物体系,应用时间毒性微板分析法系统测定3种抗生素和重金属Zn及其二元混合物射线的时间-浓度-毒性数据,以浓度加和(concentration addition,CA)与独立作用(independent action,IA)为标准加和参考模型,分析混合物毒性相互作用及其随时间变化规律。结果表明,随着暴露时间延长,3种抗生素和重金属Zn对C. pyrenoidosa的毒性逐渐增强; 2种模型对3个二元混合物体系的毒性相互作用评估基本一致,即在低浓度区域始终呈现加和作用,而在高浓度区域随暴露时间延长由协同作用逐渐转变为加和作用;而对于同一混合物体系,CA和IA模型预测毒性之间的差距随着浓度增加而增加,且IA预测曲线始终位于CA预测曲线上方,显示了IA模型在评估具有相异组分混合物的毒性时较CA模型接近实际观测值。
Contaminants commonly present in the form of mixtures in the environment,and their cumulative toxicity and toxicity interaction have potential environmental risks. Therefore,aminoglycoside antibiotics(apramycin sulfate,dihydrostreptomycin,streptomycin sulfate) and heavy metal(Zn) commonly existing in aquatic environment were selected as target contaminants,Chlorella pyrenoidosa(C. pyrenoiosa) was taken as a test organism,and a direct equipartition ray method was used to design three binary mixture systems of three antibiotics and Zn in this study. Thetime-concentration-toxicity data of the three antibiotics,heavy metal Zn and their mixture systems toward C. pyrenoiosa in different exposure time was determined using the time-dependent microplate toxicity analysis method. Concentration addition(CA) and independent action(IA) were used as the standard additive reference models to analyze toxicity interaction within mixture systems and their changings with time. The results showed that toxicity of the three antibiotics and Zn toward C. pyrenoiosa gradually increased with the lengthening of exposure time. The two models,CA and IA,were basically consistent in the assessment of the toxicity interaction within three binary mixtures,i.e.,the additive effect was always present in the low-concentration region,while the synergistic effect gradually changed to the additive effect in the high-concentration region with the extension of exposure time. For the same mixtrue system,deviations between the predicted toxicity by CA and IA models increased with the increasing of concentration. The predicted curves by IA were always above those predicted by CA,which indicated the toxicity predicted by IA was more accurate than that predicted by CA when assessing mixtures with different modes of action.
Contaminants commonly present in the form of mixtures in the environment,and their cumulative toxicity and toxicity interaction have potential environmental risks. Therefore,aminoglycoside antibiotics(apramycin sulfate,dihydrostreptomycin,streptomycin sulfate) and heavy metal(Zn) commonly existing in aquatic environment were selected as target contaminants,Chlorella pyrenoidosa(C. pyrenoiosa) was taken as a test organism,and a direct equipartition ray method was used to design three binary mixture systems of three antibiotics and Zn in this study. Thetime-concentration-toxicity data of the three antibiotics,heavy metal Zn and their mixture systems toward C. pyrenoiosa in different exposure time was determined using the time-dependent microplate toxicity analysis method. Concentration addition(CA) and independent action(IA) were used as the standard additive reference models to analyze toxicity interaction within mixture systems and their changings with time. The results showed that toxicity of the three antibiotics and Zn toward C. pyrenoiosa gradually increased with the lengthening of exposure time. The two models,CA and IA,were basically consistent in the assessment of the toxicity interaction within three binary mixtures,i.e.,the additive effect was always present in the low-concentration region,while the synergistic effect gradually changed to the additive effect in the high-concentration region with the extension of exposure time. For the same mixtrue system,deviations between the predicted toxicity by CA and IA models increased with the increasing of concentration. The predicted curves by IA were always above those predicted by CA,which indicated the toxicity predicted by IA was more accurate than that predicted by CA when assessing mixtures with different modes of action.
引文
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[3]Botero-Coy A M,Martinez-Pachon D,Boix C,et al.An investigation into the occurrence and removal of pharmaceuticals in Colombian wastewater[J].Science of the Total Environment,2018,642:842-853
[4]Liu Y,Gao B,Yue Q,et al.Influences of two antibiotic contaminants on the production,release and toxicity of microcystins[J].Ecotoxicology&Environmental Safety,2012,77(9):79-87
[5]Heberer T.Occurrence,fate,and removal of pharmaceutical residues in the aquatic environment:A review of recent research data[J].Toxicology Letters,2002,131(1):5-17
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[7]董欣琦，陈敏，张瑾，等．氨基糖苷类抗生素混合物对蛋白核小球藻的时间依赖毒性[J]．安徽建筑大学学报，2016,24(6):67-73Dong X Q,Chen M,Zhang J,et al.Time-dependent toxicity of aminoglycoside antibiotics to Chlorella pyrenoidosa[J].Journal of Anhui Jianzhu University,2016,24(6):67-73(in Chinese)
[8]Bohm D A,Stachel C S,Gowik P.Confirmatory method for the determination of streptomycin and dihydrostreptomycin in honey by LC-MS/MS[J].Food Additives&Contaminants,2012,29(2):189-196
[9]Bhat R,Gómez-López V M.Heavy Metal Contamination as a Global Problem and the Need for Prevention/Reduction Measurements[M].John Wiley&Sons,Ltd,2014:257-280
[10]Pan K,Wang W X.Trace metal contamination in estuarine and coastal environments in China[J].Science of the Total Environment,2012,421-422(3):3-16
[11]Islam M S,Ahmed M K,Habibullah-Al-Mamun M,et al.Assessment of trace metals in fish species of urban rivers in Bangladesh and health implications[J].Environmental Toxicology&Pharmacology,2015,39(1):347-357
[12]郑桂红，唐玲玲，孙建梅，等．重金属锌对锦鲤组织氧化损伤的作用[J]．江苏农业科学，2014,42(3):187-189Zheng G H,Tang L L,Sun J M,et al.Oxidative damage of heavy metal zinc to Cryprinus carpiod tissue[J].Jiangsu Agricultural Sciences,2014,42(3):187-189(in Chinese)
[13]刘树深，张瑾，张亚辉，等．APTox:化学混合物毒性评估与预测[J]．化学学报，2012,70(14):1511-1517Liu S S,Zhang J,Zhang Y H,et al.APTox:Assessment and prediction on toxicity of chemical mixtures[J].Acta Chimica Sinica,2012,70(14):1511-1517(in Chinese)
[14]Chiang Y W,Santos R M,Ghyselbrecht K,et al.Strategic selection of an optimal sorbent mixture for in-situ remediation of heavy metal contaminated sediments:Framework and case study[J].Journal of Environmental Management,2012,105(3):1-11
[15]朱骏，黄洋，赵浩，等．硝基苯及其主要降解中间产物对发光菌联合急性毒性的影响[J]．上海交通大学学报，2010,44(11):1556-1560Zhu J,Huang Y,Zhao H,et al.Joint toxicity of nitrobenzene and intermediate products to Photobacterium phosphoreum[J].Journal of Shanghai Jiaotong University,2010,44(11):1556-1560(in Chinese)
[16]刘雪，刘树深，刘海玲．构建三元混合污染物的三维等效图[J]．环境科学，2015,36(12):4574-4581Liu X,Liu S S,Liu H L.Construction of the three-dimensional isobologram for ternary pollutant mixtures[J].Acta Scientiae Circumstantiae,2015,36(12):4574-4581(in Chinese)
[17]宋晓青，刘树深，刘海玲，等．部分除草剂与重金属混合物对发光菌的毒性[J]．生态毒理学报，2008,3(3):237-243Song X Q,Liu S S,Liu H L,et al.Mixture toxicity of herbicides and heavy metal compounds to photobacteria(Vibrio qinghaiensis sp.-Q67)[J].Asian Journal of Ecotoxicology,2008,3(3):237-243(in Chinese)
[18]Huang W Y,Liu F,Liu S S,et al.Predicting mixture toxicity of seven phenolic compounds with similar and dissimilar action mechanisms to Vibrio qinghaiensis sp.nov.Q67[J].Ecotoxicology&Environmental Safety,2011,74(6):1600-1606
[19]潘永正，孙昊宇，王大力，等．混合污染物联合毒性评价模型曲线和实际浓度效应曲线之间交叉现象的研究进展[J]．生态毒理学报，2017,12(3):72-85Pan Y Z,Sun H Y,Wang D L,et al.Progress in researches on cross phenomenon between evaluation model curve and actual concentration-response curve of mixture pollutants[J].Asian Journal of Ecotoxicology,2017,12(3):72-85(in Chinese)
[20]刘树深，刘玲，陈浮．浓度加和模型在化学混合物毒性评估中的应用[J]．化学学报，2013,71(10):1335-1340Liu S S,Liu L,Chen F.Application of the concentration addition model in the assessment of chemical mixture toxicity[J].Acta Chimica Sinica,2013,71(10):1335-1340(in Chinese)
[21]Dou R N,Liu S S,Mo L Y,et al.A novel direct equipartition ray design(EquRay)procedure for toxicity interaction between ionic liquid and dichlorvos[J].Environmental Science and Pollution Research International,2011,18(5):734-742
[22]袁静，刘树深，王丽娟，等．蛋白核小球藻(Chlorella pyrenoidosa)微板毒性分析方法优化[J]．环境科学研究，2011,24(5):553-558Yuan J,Liu S S,Wang L J,et al.Optimization of microplate toxicity analysis method based on Cholrella pyrenoidose[J].Research of Environmental Sciences,2011,24(5):553-558(in Chinese)
[23]陈琼，张瑾，李小猛，等．几种抗生素对蛋白核小球藻的时间毒性微板分析法[J]．生态毒理学报，2015,10(2):190-197Chen Q,Zhang J,Li X M,et al.Time-dependent microplate toxicity analysis(T-MTA)of several antibiotics toChlorella pyrenoidosa[J].Asian Journal of Ecotoxicology,2015,10(2):190-197(in Chinese)
[24]陈敏，董欣琪，班龙科，等．多元抗生素与重金属混合物对蛋白核小球藻的时间依赖性协同与拮抗作用[J]．农业环境科学学报，2018,37(5):850-859Chen M,Dong X Q,Ban L K,et al.Time-dependent synergism and antagonism within multi-component mixtures of heavy metals and antibiotics towards Chlorella pyrenoidosa[J].Journal of Agro-Environment Science,2018,37(5):850-859(in Chinese)
[25]陈敏．抗生素与重金属混合物对蛋白核小球藻的时间依赖毒性作用研究[D]．合肥:安徽建筑大学，2017:12-13Chen M.Study on the time-dependent toxicity interaction within mixtures of antibiotics and heavy metals to Chlorella pyrenoidosa[D].Hefei:Anhui Jianzhu University,2017:12-13(in Chinese)
[26]覃礼堂，刘树深，莫凌云．改进的整合加和模型INF-CIM及其应用于混合物毒性预测[J]．中国环境科学，2014,34(7):1890-1896Qin L T,Liu S S,Mo L Y.Improved integrated addition model INFCIM and its application on prediction of mixture toxicity[J].China Environmental Science,2014,34(7):1890-1896(in Chinese)
[27]Qin L T,Liu S S,Zhang J,et al.A novel model integrated concentration addition with independent action for the prediction of toxicity of multi-component mixture[J].Toxicology,2011,280(3):164-172
[28]张帅帅．8种双酚A类化合物对MCF-7细胞的毒性及损伤研究[D]．重庆:西南大学，2012:7-8Zhang S S.Toxicity and injury research of eight bisphenol A analogues to the MCF-7 human breast carcinoma cell line[D].Chongqing:Southwest University,2012:7-8(in Chinese)
[29]Qin L T,Liu S S,Liu H L,et al.Support vector regression and least squares support vector regression for hormetic dose-response curves fitting[J].Chemosphere,2010,78(3):327-334
[30]Zhang J,Liu S S,Dou R N,et al.Evaluation on the toxicity of ionic liquid mixture with antagonism and synergism to Vibrio qinghaiensis sp.-Q67[J].Chemosphere,2011,82(7):1024-1029
[2]Jjemba P K.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,2002,93(1):267-278
[3]Botero-Coy A M,Martinez-Pachon D,Boix C,et al.An investigation into the occurrence and removal of pharmaceuticals in Colombian wastewater[J].Science of the Total Environment,2018,642:842-853
[4]Liu Y,Gao B,Yue Q,et al.Influences of two antibiotic contaminants on the production,release and toxicity of microcystins[J].Ecotoxicology&Environmental Safety,2012,77(9):79-87
[5]Heberer T.Occurrence,fate,and removal of pharmaceutical residues in the aquatic environment:A review of recent research data[J].Toxicology Letters,2002,131(1):5-17
[6]Costanzo S D,Murby J,Bates J.Ecosystem response to antibiotics entering the aquatic environment[J].Marine Pollution Bulletin,2005,51(1):218-223
[7]董欣琦，陈敏，张瑾，等．氨基糖苷类抗生素混合物对蛋白核小球藻的时间依赖毒性[J]．安徽建筑大学学报，2016,24(6):67-73Dong X Q,Chen M,Zhang J,et al.Time-dependent toxicity of aminoglycoside antibiotics to Chlorella pyrenoidosa[J].Journal of Anhui Jianzhu University,2016,24(6):67-73(in Chinese)
[8]Bohm D A,Stachel C S,Gowik P.Confirmatory method for the determination of streptomycin and dihydrostreptomycin in honey by LC-MS/MS[J].Food Additives&Contaminants,2012,29(2):189-196
[9]Bhat R,Gómez-López V M.Heavy Metal Contamination as a Global Problem and the Need for Prevention/Reduction Measurements[M].John Wiley&Sons,Ltd,2014:257-280
[10]Pan K,Wang W X.Trace metal contamination in estuarine and coastal environments in China[J].Science of the Total Environment,2012,421-422(3):3-16
[11]Islam M S,Ahmed M K,Habibullah-Al-Mamun M,et al.Assessment of trace metals in fish species of urban rivers in Bangladesh and health implications[J].Environmental Toxicology&Pharmacology,2015,39(1):347-357
[12]郑桂红，唐玲玲，孙建梅，等．重金属锌对锦鲤组织氧化损伤的作用[J]．江苏农业科学，2014,42(3):187-189Zheng G H,Tang L L,Sun J M,et al.Oxidative damage of heavy metal zinc to Cryprinus carpiod tissue[J].Jiangsu Agricultural Sciences,2014,42(3):187-189(in Chinese)
[13]刘树深，张瑾，张亚辉，等．APTox:化学混合物毒性评估与预测[J]．化学学报，2012,70(14):1511-1517Liu S S,Zhang J,Zhang Y H,et al.APTox:Assessment and prediction on toxicity of chemical mixtures[J].Acta Chimica Sinica,2012,70(14):1511-1517(in Chinese)
[14]Chiang Y W,Santos R M,Ghyselbrecht K,et al.Strategic selection of an optimal sorbent mixture for in-situ remediation of heavy metal contaminated sediments:Framework and case study[J].Journal of Environmental Management,2012,105(3):1-11
[15]朱骏，黄洋，赵浩，等．硝基苯及其主要降解中间产物对发光菌联合急性毒性的影响[J]．上海交通大学学报，2010,44(11):1556-1560Zhu J,Huang Y,Zhao H,et al.Joint toxicity of nitrobenzene and intermediate products to Photobacterium phosphoreum[J].Journal of Shanghai Jiaotong University,2010,44(11):1556-1560(in Chinese)
[16]刘雪，刘树深，刘海玲．构建三元混合污染物的三维等效图[J]．环境科学，2015,36(12):4574-4581Liu X,Liu S S,Liu H L.Construction of the three-dimensional isobologram for ternary pollutant mixtures[J].Acta Scientiae Circumstantiae,2015,36(12):4574-4581(in Chinese)
[17]宋晓青，刘树深，刘海玲，等．部分除草剂与重金属混合物对发光菌的毒性[J]．生态毒理学报，2008,3(3):237-243Song X Q,Liu S S,Liu H L,et al.Mixture toxicity of herbicides and heavy metal compounds to photobacteria(Vibrio qinghaiensis sp.-Q67)[J].Asian Journal of Ecotoxicology,2008,3(3):237-243(in Chinese)
[18]Huang W Y,Liu F,Liu S S,et al.Predicting mixture toxicity of seven phenolic compounds with similar and dissimilar action mechanisms to Vibrio qinghaiensis sp.nov.Q67[J].Ecotoxicology&Environmental Safety,2011,74(6):1600-1606
[19]潘永正，孙昊宇，王大力，等．混合污染物联合毒性评价模型曲线和实际浓度效应曲线之间交叉现象的研究进展[J]．生态毒理学报，2017,12(3):72-85Pan Y Z,Sun H Y,Wang D L,et al.Progress in researches on cross phenomenon between evaluation model curve and actual concentration-response curve of mixture pollutants[J].Asian Journal of Ecotoxicology,2017,12(3):72-85(in Chinese)
[20]刘树深，刘玲，陈浮．浓度加和模型在化学混合物毒性评估中的应用[J]．化学学报，2013,71(10):1335-1340Liu S S,Liu L,Chen F.Application of the concentration addition model in the assessment of chemical mixture toxicity[J].Acta Chimica Sinica,2013,71(10):1335-1340(in Chinese)
[21]Dou R N,Liu S S,Mo L Y,et al.A novel direct equipartition ray design(EquRay)procedure for toxicity interaction between ionic liquid and dichlorvos[J].Environmental Science and Pollution Research International,2011,18(5):734-742
[22]袁静，刘树深，王丽娟，等．蛋白核小球藻(Chlorella pyrenoidosa)微板毒性分析方法优化[J]．环境科学研究，2011,24(5):553-558Yuan J,Liu S S,Wang L J,et al.Optimization of microplate toxicity analysis method based on Cholrella pyrenoidose[J].Research of Environmental Sciences,2011,24(5):553-558(in Chinese)
[23]陈琼，张瑾，李小猛，等．几种抗生素对蛋白核小球藻的时间毒性微板分析法[J]．生态毒理学报，2015,10(2):190-197Chen Q,Zhang J,Li X M,et al.Time-dependent microplate toxicity analysis(T-MTA)of several antibiotics toChlorella pyrenoidosa[J].Asian Journal of Ecotoxicology,2015,10(2):190-197(in Chinese)
[24]陈敏，董欣琪，班龙科，等．多元抗生素与重金属混合物对蛋白核小球藻的时间依赖性协同与拮抗作用[J]．农业环境科学学报，2018,37(5):850-859Chen M,Dong X Q,Ban L K,et al.Time-dependent synergism and antagonism within multi-component mixtures of heavy metals and antibiotics towards Chlorella pyrenoidosa[J].Journal of Agro-Environment Science,2018,37(5):850-859(in Chinese)
[25]陈敏．抗生素与重金属混合物对蛋白核小球藻的时间依赖毒性作用研究[D]．合肥:安徽建筑大学，2017:12-13Chen M.Study on the time-dependent toxicity interaction within mixtures of antibiotics and heavy metals to Chlorella pyrenoidosa[D].Hefei:Anhui Jianzhu University,2017:12-13(in Chinese)
[26]覃礼堂，刘树深，莫凌云．改进的整合加和模型INF-CIM及其应用于混合物毒性预测[J]．中国环境科学，2014,34(7):1890-1896Qin L T,Liu S S,Mo L Y.Improved integrated addition model INFCIM and its application on prediction of mixture toxicity[J].China Environmental Science,2014,34(7):1890-1896(in Chinese)
[27]Qin L T,Liu S S,Zhang J,et al.A novel model integrated concentration addition with independent action for the prediction of toxicity of multi-component mixture[J].Toxicology,2011,280(3):164-172
[28]张帅帅．8种双酚A类化合物对MCF-7细胞的毒性及损伤研究[D]．重庆:西南大学，2012:7-8Zhang S S.Toxicity and injury research of eight bisphenol A analogues to the MCF-7 human breast carcinoma cell line[D].Chongqing:Southwest University,2012:7-8(in Chinese)
[29]Qin L T,Liu S S,Liu H L,et al.Support vector regression and least squares support vector regression for hormetic dose-response curves fitting[J].Chemosphere,2010,78(3):327-334
[30]Zhang J,Liu S S,Dou R N,et al.Evaluation on the toxicity of ionic liquid mixture with antagonism and synergism to Vibrio qinghaiensis sp.-Q67[J].Chemosphere,2011,82(7):1024-1029
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