环丙沙星在污水处理过程中的迁移转化及对污水生物处理的影响
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摘要
环丙沙星(Ciprofloxacin,CIP)是一种被广泛用于人类医学和动物疾病预防的抗生素类药物,在自然环境中普遍存在,以前的研究主要集中在采用不同方式对环境介质中的CIP进行吸附降解及CIP的药物作用上,有关其在污水处理过程中的迁移转化及对污水生物处理的影响尚不得而知.基于此,本文通过CIP在活性污泥处理污水中的迁移转化实验,解析其对污水生物处理过程的影响.实验结果表明:CIP的去除途径主要为生物吸附,且对低浓度CIP(0.003、0.03和0.3 mg·L~(-1))有较好的吸附效果,但高浓度CIP(3和6 mg·L~(-1))很难被去除;CIP短期/长期暴露对污泥活性及污泥生物细胞完整性无显著影响,但长期暴露会显著提高活性污泥沉降性能,同时会降低生物脱氮除磷的效率.CIP(0.05、0.5、5 mg·L~(-1))的存在使磷的去除率从97.1%±1.2%分别下降到95.8%±0.9%、89.1%±0.6%和74.3%±0.7%,出水中氨氮的去除率从96.1%±1.1%分别下降到94.6%±0.8%、87.9%±0.4%和70.2%±0.6%.机理实验表明,CIP通过抑制好氧阶段和缺氧阶段胞内聚合物聚羟基脂肪酸酯和糖原的转化来抑制磷的吸收和反硝化过程,这是CIP影响生物脱氮除磷的重要原因.此外,亚硝酸盐还原酶和多磷酸激酶的活性也受到CIP的抑制.
Ciprofloxacin(CIP) is a kind of antibiotic drugs which is widely used in human medicine and animal disease prevention. Previous investigations mainly focused on the adsorption and degradation of CIP in environmental media with different ways and the drug action of CIP, but the transformation of CIP in wastewater treatment and its impact on wastewater treatment is unknown. Therefore, this study explored the transformation of CIP in activated sludge treatment wastewater, and analyzed its effect on wastewater biological treatment process. Experimental results showed that CIP was mainly removed by biosorption, with good adsorption being observed at low CIP concentrations(0.003, 0.03 and 0.3 mg·L~(-1)). However, the biosorption performance was deteriorated at high CIP concentrations(3 and 6 mg·L~(-1)). CIP had no adverse effects on sludge viability and integrity in either short or long-term exposure, but long-term exposure significantly improved the sedimentation performance of activated sludge and decreased the efficiency of biological nitrogen and phosphorus removal. When CIP exposure levels was from 0 to 5 mg·L~(-1)(0.05, 0.5, 5 mg·L~(-1)), the removal efficiency of phosphorus was reduced from 97.1%±1.2% to 95.8%±0.9%, 89.1%±0.6% and 74.3%±0.7%, and the removal efficiency of nitrogen was decreased from 96.1%±1.1% to 94.6%±0.8%, 87.9%±0.4% and 70.2%±0.6%, respectively. The mechanism study showed that CIP suppressed phosphorus uptake and denitrification processes by inhibiting the conversion of intracellular polyhydroxyalkanoates(PHA) and glycogen in the aerobic and anoxic phases, which is an important reason for CIP affecting biological nitrogen and phosphorus removal. In addition, the activities of nitrite reductase and polyphosphate kinase were inhibited by CIP as well.
Ciprofloxacin(CIP) is a kind of antibiotic drugs which is widely used in human medicine and animal disease prevention. Previous investigations mainly focused on the adsorption and degradation of CIP in environmental media with different ways and the drug action of CIP, but the transformation of CIP in wastewater treatment and its impact on wastewater treatment is unknown. Therefore, this study explored the transformation of CIP in activated sludge treatment wastewater, and analyzed its effect on wastewater biological treatment process. Experimental results showed that CIP was mainly removed by biosorption, with good adsorption being observed at low CIP concentrations(0.003, 0.03 and 0.3 mg·L~(-1)). However, the biosorption performance was deteriorated at high CIP concentrations(3 and 6 mg·L~(-1)). CIP had no adverse effects on sludge viability and integrity in either short or long-term exposure, but long-term exposure significantly improved the sedimentation performance of activated sludge and decreased the efficiency of biological nitrogen and phosphorus removal. When CIP exposure levels was from 0 to 5 mg·L~(-1)(0.05, 0.5, 5 mg·L~(-1)), the removal efficiency of phosphorus was reduced from 97.1%±1.2% to 95.8%±0.9%, 89.1%±0.6% and 74.3%±0.7%, and the removal efficiency of nitrogen was decreased from 96.1%±1.1% to 94.6%±0.8%, 87.9%±0.4% and 70.2%±0.6%, respectively. The mechanism study showed that CIP suppressed phosphorus uptake and denitrification processes by inhibiting the conversion of intracellular polyhydroxyalkanoates(PHA) and glycogen in the aerobic and anoxic phases, which is an important reason for CIP affecting biological nitrogen and phosphorus removal. In addition, the activities of nitrite reductase and polyphosphate kinase were inhibited by CIP as well.
引文
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Babi? S,Peri?a M,?kori? I. 2013. Photolytic degradation of norfloxacin,enrofloxacin and ciprofloxacin in various aqueous media[J].Chemosphere 91:1635-1642
Chang P H,Jiang W T,Li Z,et al.2016.Interaction of ciprofloxacin and probe compounds with palygorskite PFl-1[J].Journal of Hazardous Materials,303:55-63
Chen A,Chen Y,Ding C,et al.2015.Effects of tetracycline on simultaneous biological wastewater nitrogen and phosphorus removal[J].RSC Advances,5:59326-59334
Chen H B,Wang D B,Li X M,et al.2014a.Effects of Cd(II) on wastewater biological nitrogen and phosphorus removal[J].Chemosphere, 117:27-32
Chen Y G,Wang D B,Zheng X,et al.2014b.Biological nutrient removal with low nitrous oxide generation by cancelling the anaerobic phase and extending the idle phase in a sequencing batch reactor[J].Chemosphere, 109:56-63
Chen Y,Su Y,Zheng X,et al.2012.Alumina nanoparticles-induced effects on wastewater nitrogen and phosphorus removal after short-term and long-term exposure[J].Water ResEarch,46:4379-4386
陈涛,李彦文,莫测辉,等.2010.广州污水厂磺胺和喹诺酮抗生素污染特征研究[J].环境科学与技术,33(6):150-153;186
戴琦.2017.环丙沙星废水的膜生物反应器处理特性及污泥中抗性基因的变化研究[D].上海:上海师范大学
Doorslaer X V,Dewulf J,Langenhove H V,et al.2014.Fluoroquinolone antibiotics:an emerging class of environmental micropollutants[J].Science Total Environmental,500:250-269
Girardi C,Greve J,Lamsh?ft M,et al.2011.Biodegradation of ciprofloxacin in water and soil and its effects on the microbial communities[J].Journal of Hazardous Materials,198:22-30
Golet E M,Xifra I,Siegrist H,et al.2003.Environmental exposure assessment of fluoroquinolone antibacterial agents from sewage to soil[J].Environmental Science and Technology,37:3243-3249
Golet E M,Xifra I,Siegrist H,et al.2003.Environmental exposure assessment of fluoroquinolone antibacterial agents from sewage to soil[J].Environmental Science and Technology,37 (15):3243-3249
Gonzalez-Pleiter M,Gonzalo S,Rodea-Palomares I,et al.2013.Toxicity of five antibiotics and their mixtures towards photosynthetic aquatic organisms:implications for environmental risk assessment[J].Water Research,47 (6):2050-2064
Guo J,Li J,Chen H,et al.2017.Metagenomic analysis reveals wastewater treatment plants as hotspots of antibiotic resistance genes and mobile genetic elements[J].Water Research,123:468-478
葛伟丽.2014.长期施用鸡粪农田土壤中典型抗生素耐药细菌及其抗性基因污染分析[D].泰安:山东农业大学
何势.2016.曝气生物滤池中环丙沙星去除行为及其对降解菌群抗药性的诱导作用[D].上海:东华大学
邰义萍,莫测辉,李彦文,等.2010.长期施用粪肥土壤中喹诺酮类抗生素的含量与分布特征[J].中国环境科学,30(6):816-821
Ji Y,Ferronatope C,Salvador A,et al.2014.Degradation of ciprofloxacin and sulfamethoxazole by ferrous-activated rsulfate:implications for remediation of groundwater contaminated by antibiotics[J].Science of the Total Environment,472:800-808
Karthik K G,Meyer M T.2006.Occurrence of antibiotics in wastewater treatment facilities in Wisconsin,USA[J].Science of the Total Environment,361(1/2/3):196-207
Leal R M P,Figueira R F,Tornisielo V L,et al.2012.Occurrence and sorption of fluoroquinolones in poultry litters and soils from S?o Paulo State,Brazil[J].Science of the Total Environment,432:344-349
Li B,Zhang T.2010.Biodegradation and adsorption of antibiotics in the activated sludge process[J].Environmental Science and Technology,44:3468-3473
Lindberg R H,Olofsson U,Rendahl P,et al.2006.Behavior of fluoroquinolones and trimethoprim during mechanical,chemical,and active sludge treatment of sewage water and digestion of sludge[J].Environmental Science and Technology,40:1042-1048
Lindberg R H,Wennberg P,Johansson M I,et al.2005.Screening of human antibiotic substances and determination of weekly mass flows in five sewage treatment plants in Sweden[J].Environmental Science and Technology,39(10):3421-3429
Louvet J N,Giammarino C,Potier O,et al.2010.Adverse effects of erythromycin on the structure and chemistry of activated sludge[J].Environmental PollutIon,158:688-693
Mosmann T.1983.Rapid colorimetric assay for cellular growth and survival:application to proliferation and cytotoxicity 362 assays[J].Journal of Immunological Methods,65:55-63
Mougin C,Cheviron N,Repincay C,et al.2013.Earthworms highly increase ciprofloxacin mineralization in soils[J].Environmental Chemistry Letters,11:127-133
Pijuan M,Ye L,Yuan Z.2010.Free nitrous acid inhibition on the aerobic metabolism of poly-phosphate accumulating organisms[J].Water Research,44:6063-6072
Rosal R,Rodríguez A,Perdigón-Melón J A,et al.2010.Occurrence of emerging pollutants in urban wastewater and their removal through biological treatment followed by ozonation[J].Water Research,44(2):578-588
Sapkota A R,Curriero F C,Gibson K E,et al.2007.Antibioticresistant enterococci and fecal indicators in surface water and groundwater impacted by a concentrated Swine feeding operation[J].Environmental Health Perspectives,115(7):1040-1045
Suarez S,Carballa M,Omil F,et al.2008.How are pharmaceutical andpersonal care products (PPCPs) removed from urban wastewaters[J].Reviews in Environmental Science and Biotechnology,7(2):125-138
Tong L,Li P,Wang Y X,et al.2009.Analysis of veterinary antibiotic residues in swine wastewater and environmental water samples using optimized SPE-LC/MS/MS[J].Chemosphere,74(8):1090-1097
Tsai Y P,Tzeng H F,Lin J W,et al.2013.Verification of enzymes deterioration due to Cu(II) presence in an enhanced biological phosphorus removal system[J].Chemosphere,91:602-607
Vieno N,Tuhkanen T,Kronberg L.2007.Elimination of pharmaceuticals in sewage treatment plants in Finland[J].Water Research,41(5):1001-1012
Wang D B,Zheng W,Liao D,et al.2013a.Effect of initial pH control on biological phosphorus removal induced by the aerobic/extended-idle regime[J].Chemosphere,90:2279-2287
Wang D B,Zheng W,Li X M,et al.2013b.Evaluation of the feasibility of alcohols serving as external carbon sources for biological phosphorus removal induced by the oxic/extended-idle regime[J].Biotechnology & Bioengineering,110(3):827-837
Wang D B,Xu Q X,Yang W Q,et al.2014.A new configuration of sequencing batch reactor operated as amodified aerobic/extended-idle regime for simultaneously saving reactor volume and enhancing biological phosphorus removal[J].Biochemical Engineering Journal,87:15-24
王佳宁,徐永平,李晓宇,等.2017.畜禽粪便抗生素残留及其对环境的影响[J].畜牧与兽医,49(10):140-144
王桥军,亦如瀚,莫测辉,等.2009.广州市水环境中喹诺酮类抗生素的污染特性[J].生态科学,28(3):276-280
Wolfson J S,Hooper D C.1985.The fluoroquinolones: Structures, mechanisms of action and resistance, and spectra of activity in vitro[J].Antimicrobial Agents and Chemotherapy,28(4):581-586
Wright G D.2005.Bacterial resistance to antibiotics:enzymatic degradation and modification[J].Advanced Drug Delivery Reviews,57 (10):1451-1470
Wu C,Spongberg A L,Witter J D.2009.Sorption and biodegradation of selected antibiotics in biosolids[J].J Environ Sci Health A,44(5):454-461
Zhang Y P,Ma X G,Fan Y M.2014.A rapid and sensitive method for determination of melamine in fish,shrimp,clam,and winkle by gas chromatography-mass spectrometry with microwave-assisted derivatization[J].Food Analytical Methods,7(9):1763-1769
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 and Technology,49(11):6772-6782
Babi? S,Peri?a M,?kori? I. 2013. Photolytic degradation of norfloxacin,enrofloxacin and ciprofloxacin in various aqueous media[J].Chemosphere 91:1635-1642
Chang P H,Jiang W T,Li Z,et al.2016.Interaction of ciprofloxacin and probe compounds with palygorskite PFl-1[J].Journal of Hazardous Materials,303:55-63
Chen A,Chen Y,Ding C,et al.2015.Effects of tetracycline on simultaneous biological wastewater nitrogen and phosphorus removal[J].RSC Advances,5:59326-59334
Chen H B,Wang D B,Li X M,et al.2014a.Effects of Cd(II) on wastewater biological nitrogen and phosphorus removal[J].Chemosphere, 117:27-32
Chen Y G,Wang D B,Zheng X,et al.2014b.Biological nutrient removal with low nitrous oxide generation by cancelling the anaerobic phase and extending the idle phase in a sequencing batch reactor[J].Chemosphere, 109:56-63
Chen Y,Su Y,Zheng X,et al.2012.Alumina nanoparticles-induced effects on wastewater nitrogen and phosphorus removal after short-term and long-term exposure[J].Water ResEarch,46:4379-4386
陈涛,李彦文,莫测辉,等.2010.广州污水厂磺胺和喹诺酮抗生素污染特征研究[J].环境科学与技术,33(6):150-153;186
戴琦.2017.环丙沙星废水的膜生物反应器处理特性及污泥中抗性基因的变化研究[D].上海:上海师范大学
Doorslaer X V,Dewulf J,Langenhove H V,et al.2014.Fluoroquinolone antibiotics:an emerging class of environmental micropollutants[J].Science Total Environmental,500:250-269
Girardi C,Greve J,Lamsh?ft M,et al.2011.Biodegradation of ciprofloxacin in water and soil and its effects on the microbial communities[J].Journal of Hazardous Materials,198:22-30
Golet E M,Xifra I,Siegrist H,et al.2003.Environmental exposure assessment of fluoroquinolone antibacterial agents from sewage to soil[J].Environmental Science and Technology,37:3243-3249
Golet E M,Xifra I,Siegrist H,et al.2003.Environmental exposure assessment of fluoroquinolone antibacterial agents from sewage to soil[J].Environmental Science and Technology,37 (15):3243-3249
Gonzalez-Pleiter M,Gonzalo S,Rodea-Palomares I,et al.2013.Toxicity of five antibiotics and their mixtures towards photosynthetic aquatic organisms:implications for environmental risk assessment[J].Water Research,47 (6):2050-2064
Guo J,Li J,Chen H,et al.2017.Metagenomic analysis reveals wastewater treatment plants as hotspots of antibiotic resistance genes and mobile genetic elements[J].Water Research,123:468-478
葛伟丽.2014.长期施用鸡粪农田土壤中典型抗生素耐药细菌及其抗性基因污染分析[D].泰安:山东农业大学
何势.2016.曝气生物滤池中环丙沙星去除行为及其对降解菌群抗药性的诱导作用[D].上海:东华大学
邰义萍,莫测辉,李彦文,等.2010.长期施用粪肥土壤中喹诺酮类抗生素的含量与分布特征[J].中国环境科学,30(6):816-821
Ji Y,Ferronatope C,Salvador A,et al.2014.Degradation of ciprofloxacin and sulfamethoxazole by ferrous-activated rsulfate:implications for remediation of groundwater contaminated by antibiotics[J].Science of the Total Environment,472:800-808
Karthik K G,Meyer M T.2006.Occurrence of antibiotics in wastewater treatment facilities in Wisconsin,USA[J].Science of the Total Environment,361(1/2/3):196-207
Leal R M P,Figueira R F,Tornisielo V L,et al.2012.Occurrence and sorption of fluoroquinolones in poultry litters and soils from S?o Paulo State,Brazil[J].Science of the Total Environment,432:344-349
Li B,Zhang T.2010.Biodegradation and adsorption of antibiotics in the activated sludge process[J].Environmental Science and Technology,44:3468-3473
Lindberg R H,Olofsson U,Rendahl P,et al.2006.Behavior of fluoroquinolones and trimethoprim during mechanical,chemical,and active sludge treatment of sewage water and digestion of sludge[J].Environmental Science and Technology,40:1042-1048
Lindberg R H,Wennberg P,Johansson M I,et al.2005.Screening of human antibiotic substances and determination of weekly mass flows in five sewage treatment plants in Sweden[J].Environmental Science and Technology,39(10):3421-3429
Louvet J N,Giammarino C,Potier O,et al.2010.Adverse effects of erythromycin on the structure and chemistry of activated sludge[J].Environmental PollutIon,158:688-693
Mosmann T.1983.Rapid colorimetric assay for cellular growth and survival:application to proliferation and cytotoxicity 362 assays[J].Journal of Immunological Methods,65:55-63
Mougin C,Cheviron N,Repincay C,et al.2013.Earthworms highly increase ciprofloxacin mineralization in soils[J].Environmental Chemistry Letters,11:127-133
Pijuan M,Ye L,Yuan Z.2010.Free nitrous acid inhibition on the aerobic metabolism of poly-phosphate accumulating organisms[J].Water Research,44:6063-6072
Rosal R,Rodríguez A,Perdigón-Melón J A,et al.2010.Occurrence of emerging pollutants in urban wastewater and their removal through biological treatment followed by ozonation[J].Water Research,44(2):578-588
Sapkota A R,Curriero F C,Gibson K E,et al.2007.Antibioticresistant enterococci and fecal indicators in surface water and groundwater impacted by a concentrated Swine feeding operation[J].Environmental Health Perspectives,115(7):1040-1045
Suarez S,Carballa M,Omil F,et al.2008.How are pharmaceutical andpersonal care products (PPCPs) removed from urban wastewaters[J].Reviews in Environmental Science and Biotechnology,7(2):125-138
Tong L,Li P,Wang Y X,et al.2009.Analysis of veterinary antibiotic residues in swine wastewater and environmental water samples using optimized SPE-LC/MS/MS[J].Chemosphere,74(8):1090-1097
Tsai Y P,Tzeng H F,Lin J W,et al.2013.Verification of enzymes deterioration due to Cu(II) presence in an enhanced biological phosphorus removal system[J].Chemosphere,91:602-607
Vieno N,Tuhkanen T,Kronberg L.2007.Elimination of pharmaceuticals in sewage treatment plants in Finland[J].Water Research,41(5):1001-1012
Wang D B,Zheng W,Liao D,et al.2013a.Effect of initial pH control on biological phosphorus removal induced by the aerobic/extended-idle regime[J].Chemosphere,90:2279-2287
Wang D B,Zheng W,Li X M,et al.2013b.Evaluation of the feasibility of alcohols serving as external carbon sources for biological phosphorus removal induced by the oxic/extended-idle regime[J].Biotechnology & Bioengineering,110(3):827-837
Wang D B,Xu Q X,Yang W Q,et al.2014.A new configuration of sequencing batch reactor operated as amodified aerobic/extended-idle regime for simultaneously saving reactor volume and enhancing biological phosphorus removal[J].Biochemical Engineering Journal,87:15-24
王佳宁,徐永平,李晓宇,等.2017.畜禽粪便抗生素残留及其对环境的影响[J].畜牧与兽医,49(10):140-144
王桥军,亦如瀚,莫测辉,等.2009.广州市水环境中喹诺酮类抗生素的污染特性[J].生态科学,28(3):276-280
Wolfson J S,Hooper D C.1985.The fluoroquinolones: Structures, mechanisms of action and resistance, and spectra of activity in vitro[J].Antimicrobial Agents and Chemotherapy,28(4):581-586
Wright G D.2005.Bacterial resistance to antibiotics:enzymatic degradation and modification[J].Advanced Drug Delivery Reviews,57 (10):1451-1470
Wu C,Spongberg A L,Witter J D.2009.Sorption and biodegradation of selected antibiotics in biosolids[J].J Environ Sci Health A,44(5):454-461
Zhang Y P,Ma X G,Fan Y M.2014.A rapid and sensitive method for determination of melamine in fish,shrimp,clam,and winkle by gas chromatography-mass spectrometry with microwave-assisted derivatization[J].Food Analytical Methods,7(9):1763-1769
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 and Technology,49(11):6772-6782
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