Combined toxicity of sequential exposure of antibiotics and fungicides on green algae
LI Chao-jie1, NONG Qiong-yuan1, QIN Li-tang1,2,3, MO Ling-yun2,3,4, LIANG Yan-peng1,2,3, ZENG Hong-hu1,2,3, DENG Zhen-gui5, LIU Liang5
1. College of Environmental Science and Engineering, Guilin University of Technology, Guilin 541004, China; 2. Guangxi Key Laboratory of Environmental Pollution Control Theory and Technology, Guilin University of Technology, Guilin 541004, China; 3. Collaborative Innovation Center for Water Pollution Control and Water Safety in Karst Area, Guilin University of Technology, Guilin 541004, China; 4. Technical innovation center of mine geological environment restoration engineering in Shishan area of South China, Ministry of natural resourcesn, Nanning 530022, China; 5. Hengsheng Water Environment Management Co, LTD., Guilin 541199, China
Abstract:The mixture systems of three antibiotics (doxycycline hydrochloride (DOX), erythromycin (ERY), oxytetracycline (OXY)) and three triazole fungicides (myclobutanil(MYC), propiconazole (PRO) and tebuconazole (TCZ)) were selected as target pollutants. The primary producer green algae (Chlorella pyrenoidosa) in the ecosystem was used as the test organism to study the combined toxicity of sequential exposure to target contaminants. The results showed that the inhibitory toxicities of six single target pollutants to Chlorella pyrenoidosa were: PRO>DOX>TCZ>ERY>MYC>OXY. The difference of inhibition rates between simultaneous exposure and sequential exposure of antibiotic triazole bactericide mixture system mixed at 50% effect concentration was 0.38%~36.76%. The toxicity to Chlorella pyrenoidosa increased up to 36.82% when DOX, PRO, TCZ, and MYC were exposed to Chlorella pyrenoidosa in the reverse order. Under the influence of different concentrations and time, the sequential exposure toxicities of PRO-DOX and TCZ-DOX were higher than that of DOX-PRO and DOX-TCZ after adjusting the exposure sequence. The higher concentrations the greater difference of inhibition rates. At the exposure time of 96h~144h, the difference of sequential exposure inhibition rates of exposure concentration EC50/20 was 0.65%~11.57%. The difference of sequential exposure inhibition rates of exposure concentration EC50 was 0.15%~36.93%. The range of sequential exposure inhibition rate increased with the increase of concentration. At the exposure concentration EC50/20 to EC50, the difference of sequential exposure inhibition rates of exposure time 96h was 0.29%~36.93%. The difference of sequential exposure inhibition rates of exposure time 144h was 0.215%~30.09%. The range of sequential exposure inhibition rate decreased with the increase of time. Therefore, sequential exposure changed the combined toxicity of antibiotics and triazole fungicides to Chlorella pyrenoidosa. The sequential exposure, exposure time, and exposure concentration were the key factors affecting the toxicity.
李超杰, 农琼媛, 覃礼堂, 莫凌云, 梁延鹏, 曾鸿鹄, 邓振贵, 刘良. 抗生素与杀菌剂顺序暴露对绿藻的联合毒性[J]. 中国环境科学, 2023, 43(1): 404-414.
LI Chao-jie, NONG Qiong-yuan, QIN Li-tang, MO Ling-yun, LIANG Yan-peng, ZENG Hong-hu, DENG Zhen-gui, LIU Liang. Combined toxicity of sequential exposure of antibiotics and fungicides on green algae. CHINA ENVIRONMENTAL SCIENCECE, 2023, 43(1): 404-414.
王静,杨代蓉.浅谈兽用抗生素的应用现状及存在的问题[J]. 现代畜牧科技, 2018,37(5):132. Wang J, Yang D R. Application status and problems of veterinary antibiotics[J]. Modern Animal Husbandry Technology, 2018,37(5):132.
[2]
Castiglioni S, Bagnati R, Fanelli R, et al. Removal of pharmaceuticals in sewage treatment plants in Italy[J]. Environmental Science & Technology, 2006,40:357-363.
[3]
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.
[4]
吴文铸,郭敏,孔德祥,等.3种三唑类杀菌剂的环境降解特性[J]. 生态与农村环境学报, 2016,32(5):837-841. Wu W Z, Guo M, Kong D X, et al. Environmental degradation characteristics of three triazole fungicides[J]. Journal of Ecology and Rural Environment, 2016,32(5):837-841.
[5]
Tong Z, Dong X, Yang S, et al. Enantioselective effects of the chiral fungicide tetraconazole in wheat:Fungicidal activity and degradation behavior[J]. Environmental pollution, 2019,247:1-8.
[6]
宋桂芳,张世文,庄红娟,等.农用地大环内酯类抗生素与杀菌剂残留污染评价[J]. 环境化学, 2022,41(7):2309-2319. Song G F, Zhang S W, Zhuang H J, et al. Pollution assessment of macrolide antibiotics and fungicides residues in agricultural land[J]. Environmental Chemistry, 2022,41(7):2309-2319.
[7]
刘敏,覃礼堂,莫凌云,等.4种唑类杀菌剂对蛋白核小球藻的急性毒性及其致毒机理[J]. 生态毒理学报, 2021,16(4):301-312. Liu M, Qin L T, Mo L Y, et al. Acute toxicity and mechanism of four azole fungicides to Chlorella pyrenoidosa[J]. Asian Journal of Ecotoxicology, 2021,16(4):301-312.
[8]
Sui N, Zhang Z, Zhang J. Alteration between inhibition and stimulation in individual and mixture effects of[amim]Br and[apyr]Br on Aliivibrio fischeri:Time and side-chain dependence[J]. Chemosphere, 2019,233(OCT.):292-299.
[9]
Zhang J, Liu S S, Dong X Q, et al. Predictability of the time- dependent toxicities of aminoglycoside antibiotic mixtures to Vibrio qinghaiensis sp.-Q67[J]. RSC Advances, 2015,5(129):107076- 107082.
[10]
陶敏,贺锋,胡晗,等.碳氧调控下人工湿地净化效果的协同与拮抗研究[J]. 中国环境科学, 2015,35(12):3646-3652. Tao M, He F, Hu H, et al. Synergistic and antagonistic effect of treatment performance of constructed wetlands under artificial aeration and external carbon source[J]. China Environmental Science, 2015,35(12):3646-3652.
[11]
丁婷婷,董欣琪,张瑾,等.3种氨基糖苷类抗生素对水生生物的时间依赖联合毒性作用比较[J]. 生态毒理学报, 2018,13(1):126-137. Ding T T, Dong X Q, Zhang J, et al. Comparison of time-dependent joint toxicity interaction of three aminoglycosides antibiotics between two aquatic organisms[J]. Asian Journal of Ecotoxicology, 2018,13(1):126-137.
[12]
章小强,胡晓娜,陈彩东,等.镉与S-异丙甲草胺对斜生栅藻的联合毒性作用[J]. 环境科学, 2015,36(3):1069-1074. Zhang X Q, Hu X N, Chen C D, et al. Combined toxicity of cadmium and S-metolachlor to Scenedesmus obliquus [J]. Environmental Science, 2015,36(3):1069-1074.
[13]
农琼媛,覃礼堂,莫凌云,等.抗生素与三唑类杀菌剂混合物对羊角月牙藻的长期毒性相互作用研究[J]. 生态毒理学报, 2019,14(4):140-149. Nong Q Y, Qin L T, Mo L Y, et al. The toxic interactions of long-term effects involving antibiotics and triazole fungicides on Selenastrum capricornutum[J]. Asian Journal of Ecotoxicology, 2019,14(4):140- 149.
[14]
Ashauer R, Boxall A, Brown C. Modeling combined effects of pulsed exposure to carbaryl and chlorpyrifos on Gammarus pulex[J]. Environmental Science & Technology, 2007,41(15):5535-5541.
[15]
Ashauer R, O'Connor, Isabel, Escher B I. Toxic mixtures in time-the sequence makes the poison[J]. Environmental Science & Technology, 2017,51(5):3084-3092.
[16]
Russo R, Becker J M, Liess M. Sequential exposure to low levels of pesticides and temperature stress increase toxicological sensitivity of crustaceans[J]. The Science of the Total Environment, 2018,610- 611(jan.1):563-569.
[17]
Supriya B, Krutika D. The enhanced lipid productivity of Chlorella minutissima and Chlorella pyrenoidosa by carbon coupling nitrogen manipulation for biodiesel production[J]. Environmental Science and Pollution Research, 2019,26(4):3492-3500.
[18]
Mo L Y, Zheng M Y, Qin M, et al. Quantitative characterization of the toxicities of Cd-Ni and Cd-Cr binary mixtures using combination index method[J]. BioMed Research International, 2016; 2016:4158415.
[19]
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):553-558. Yuan J, Liu S S, Wang L J, et al. Optimization of microplate toxicity analysis method based on Chlorella Pyrenoidose [J]. Research of Environment Science, 2011,24(5):553-558.
[20]
Organization for Economic Co-operation and Development (OECD). Test No. 201:Alga, growth inhibition test[R]. Paris:OECD, 2006.
[21]
Qin L T, Chen Y H, Zhang X, et al. QSAR prediction of additive and non-additive mixture toxicities of antibiotics and pesticide[J]. Chemosphere, 2018,198(5):122-129.
[22]
Mo L Y, Zhao D N, Qin M, et al. Joint toxicity of six common heavy metals to Chlorella pyrenoidosa [J]. Environmental Science & Pollution Research, 2017,26(30):30554-30.
[23]
刘树深.化学混合物毒性评估与预测方法[M]. 北京:科学出版社, 2017:4-9. Liu S S. Assessment and prediction of toxicity of chemical mixtures[M]. Beijing:2017:4-9.
[24]
郑乔峰,居珍,刘树深.敌敌畏及其代谢产物对青海弧菌和秀丽线虫的联合毒性[J]. 化学学报, 2019,77(10):1008-1016. Zheng Q F, Ju Z, Liu S S. Combined toxicity of dichlorvos and its metabolites to Vibrio qinghaiensis sp.-Q67 and Caenorhabditis elegans[J]. Acta Chimica Sinica, 2019,77(10):1008-1016.
[25]
Qin L T, Zhang X, Mo L Y, et al. Further exploring linear concentration addition and independent action for predicting non- interactive mixture toxicity[J]. Chinese Journal of Structural Chemistry, 2017,36(6):886-896.
[26]
钟才高,曹壑,曾明,等.农药三唑磷和杀虫单对小鼠的联合毒作用研究[J]. 实用预防医学, 2002,9(6):613-615. Zhong C G, Cao H, Liu X M, et al. Study on the joint toxic action of pesticide triazophos and monosuitup in mice[J]. Practical Preventive M edicine, 2002,9(6):613-615.
[27]
王桂祥.低浓度混合抗生素对普通小球藻的联合毒性效应及机理[D]. 青岛:青岛科技大学, 2019:17-20. Wang G X. Combined effects and mechanisms of low concentration mixed antibiotics on Chlorella Vulgaris[D]. Qingdao:2019:17-20.
[28]
Zhang J, Yu Z Y. Transgenerational effects of different sequential exposure to 2,2',4,4'-tetra-brominated diphenyl ether (BDE47) and lead (Pb) on Caenorhabditis elegans[J]. Environmental Sciences Europe, 2020,32(1):44.
[29]
Nong Q Y, Liu Y A, Qin L T, et al. Toxic mechanism of three azole fungicides and their mixture to green alga Chlorella pyrenoidosa[J]. Chemosphere, 2020,262:127793.
[30]
Ashauer R, O'Connor I, Hintermeister A, et al. Death dilemma and organism recovery in ecotoxicology[J]. Environmental Science & Technology, 2015,49(7):10136-10146.
[31]
Li H, Zhang Q, Su H, et al. High tolerance and delayed responses of daphnia magna to neonicotinoid insecticide imidacloprid:Toxicokinetic and toxicodynamic modeling[J]. Environmental Science & Technology, 2021,55(1):458-467.
[32]
Ashauer R, Hintermeister A, Caravatti I, et al. Toxicokinetic and toxicodynamic modeling explains carry-over toxicity from exposure to diazinon by slow organism recovery[J]. Environmental Science & Technology, 2010,44(10):3963-3971.
[33]
Roman D L, Voiculescu D I, Filip M, et al. Effects of triazole fungicides on soil microbiota and on the activities of enzymes found in soil:A review[J]. Agriculture, 2021,11(9):893.
[34]
van Eijk E, Wittekoek B, Kuijper E J, et al. DNA replication proteins as potential targets for antimicrobials in drug-resistant bacterial pathogens[J]. Journal of Antimicrobial Chemotherapy, 2017,72(5):1275-1284.
[35]
Guo J, Bai Y, Chen Z, et al. Transcriptomic analysis suggests the inhibition of DNA damage repair in green alga Raphidocelis subcapitata exposed to roxithromycin[J]. Ecotoxicology and Environmental Safety, 2020,201:110737.
[36]
曹端韬.土壤中戊唑醇残留引致的烟曲霉对三唑类抗真菌药物抗药性及其机制[D]. 杭州:浙江大学, 2021:15-39. Cao D T. Resistance and its mechanisms of aspergillus fumigatus to triazole antifungal agents induced by tebuconazole in soil[D]. Hangzhou:Zhejiang University, 2021:15-39.
[37]
Sunghwan K, Chen J, Cheng T, et al. PubChem in 2021:new data content and improved web interfaces[J]. Nucleic Acids Research, 2021,49:D1388-D1395.
[38]
Lewis K A, Tzilivakis J, warner D J, et al. An international database for pesticide risk assessments and management[J]. Human and Ecological Risk Assessment:An International Journal, 2016,22(4):1050-1064.
[39]
王世豪,石明浩,刘苏.顺序暴露场景下四环素和砷对斑马鱼的联合毒性效应[J]. 环境科学学报, 2020,40(12):4590-4597. Wang S H, Shi M H, Liu S. Combined toxicity of tetracycline and arsenic on zebrafish in sequential exposure scenarios[J]. Acta Scientiae Circumstantiae, 2020,40(12):4590-4597.
[40]
薛喜枚,朱永官.土壤中砷的生物转化及砷与抗生素抗性的关联[J]. 土壤学报, 2019,56(4):763-772. Xue X M, Zhu Y G. Biotransformation of arsenic in soil and the relationship between arsenic and antibiotic resistance[J]. Journal of soil, 2019,56(4):763-772.
[41]
陈帅,邹海燕,高方舟,等.抗生素,重金属和杀生剂抗性共选择机制[J]. 生态毒理学报, 2020,15(2):1-10. Chen S, Zou H Y, Gao F Z, et al. Co-selection mechanism of antibiotic, metal and biocide resistance[J]. Asian Journal of Ecotoxicology, 2020,15(2):1-10.
[42]
Leng L J, Wei L, Xiong Q, et al. Use of microalgae based technology for the removal of antibiotics from wastewater:A review[J]. Chemosphere, 2020,238:124680.
[43]
Hena S, Gutierrez L, Croue J P. Removal of pharmaceutical and personal care products (PPCPs) from wastewater using microalgae:A review[J]. Journal of Hazardous Materials, 2020,403:124041.
[44]
Wang X, Dou X, Wu J, et al. Attenuation pathways of erythromycin and biochemical responses related to algal growth and lipid synthesis in a microalga-effluent system[J]. Environmental Research, 2021, 195(1):110873.
[45]
Xiong Q, Hu L X, Liu Y S, et al. Microalgae-based technology for antibiotics removal:From mechanisms to application of innovational hybrid systems[J]. Environment international, 2021,155:106594.