抗生素在城市污水处理过程中的去除研究进展
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摘要
抗生素是一种具有潜在生态风险的新兴污染物,其在环境水体中长期存在和积累会对受纳水生生物及人体健康产生不利影响,因此引起了全社会的广泛关注。城市污水处理厂作为水循环和污染控制的重要环节,是抗生素向环境迁移转化的重要来源。该文以8种典型抗生素为研究对象,综述了它们的物理化学性质及其在传统污水处理厂中的归趋、浓度水平以及相应的去除效率,探讨了它们的深度处理技术及其在再生水厂中的去除情况,并展望了该领域未来研究发展方向。
As a new kind of pollutant with potential ecological risks, the existence and accumulation of antibiotics in aquatic environment could cause adverse effect to the aquatic organisms and human health, which aroused wide public concern. As the important link in water cycle and pollution control, WWTPs(waste water treatment plants) are considered as the crucial source of antibiotics in waterways. This paper took eight kinds of antibiotics as research objectied to summarize their physicochemical properties, fate, concentration level and the corresponding removal efficiency, and study their advanced treatment technology and removal efficiency in reclaimed water plants, as well as looked forward to the future research and development direction of this field.
As a new kind of pollutant with potential ecological risks, the existence and accumulation of antibiotics in aquatic environment could cause adverse effect to the aquatic organisms and human health, which aroused wide public concern. As the important link in water cycle and pollution control, WWTPs(waste water treatment plants) are considered as the crucial source of antibiotics in waterways. This paper took eight kinds of antibiotics as research objectied to summarize their physicochemical properties, fate, concentration level and the corresponding removal efficiency, and study their advanced treatment technology and removal efficiency in reclaimed water plants, as well as looked forward to the future research and development direction of this field.
引文
[1]邵一如,席北斗,曹金玲,等.抗生素在城市污水处理系统中的分布及去除[J].环境科学与技术,2013,36(7):85-92.Shao Yiyu,Xi Beidou,Cao Jinling,et al.Distribution and removal of antibiotics in urban sewage treatment systems[J].Environmental Science&Technology,2013,36(7):85-92.
[2]陈栋,王烁阳,王玉玺,等.典型内分泌干扰物在城市污水处理过程中的去除研究进展[J].青岛理工大学学报,2018,39(6):1-9.Chen Dong,Wang Shuoyang,Wang Yuxi,et al.Research progress on removal of typical endocrine disruptors in urban sewage treatment[J].Journal of Qingdao Technological University,2018,39(6):1-9.
[3]Chai Y F,Zhang Y X,Chen M X,et al.Distribution and treatment effect of antibiotics of typical WWTPs in small town of China[J].Environmental Science,2018,39(6):2724-2731.
[4]Zhao X,Wang X C,Chen Z L,et al.Microbial community structure and pharmaceuticals and personal care products removal in a membrane bioreactor seeded with aerobic granular sludge[J].Applied Microbiology and Biotechnology,2015,99(1):425-433.
[5]Li W H,Shi Y L,Gao L H,et al.Occurrence and removal of antibiotics in a municipal wastewater reclamation plant in Beijing,China[J].Chemosphere,2013,92(4):435-444.
[6]Nie Y,Qiang Z,Zhang H,et al.Fate and seasonal variation of endocrine-disrupting chemicals in a sewage treatment plant with A/A/O process[J].Separation and Purification Technology,2012,84:9-15.
[7]Matos M,Pereira M A,Parpot P,et al.Influence of tetracycline on the microbial community composition and activity of nitrifying biofilms[J].Chemosphere,2014,117:295-302.
[8]Luo Y L,Guo W S,Ngo H H,et al.A review on the occurrence of micropollutants in the aquatic environment and their fate and removal during wastewater treatment[J].Science of the Total Environment,2014,473/474:619-641.
[9]Polesel F,Andersen H R,Trapp S,et al.Removal of antibiotics in biological wastewater treatment systems-a critical assessment using the activated sludge modeling framework for xenobiotics(ASM-X)[J].Environmental Science and Technology,2016,50(19):10316-10334.
[10]Gerbersdorf S U,Cimatoribus C,Class H,et al.Anthropogenic trace compounds(ATCs)in aquatic habitats-research needs on sources,fate,detection and toxicity to ensure timely elimination strategies and risk management[J].Environment International,2015,79(3):85-105.
[11]Li B,Zhang T.Biodegradation andadsorption of antibiotics in the activated sludge process[J].Environmental Science and Technology,2010,44(9):3468-3473.
[12]高俊红,王兆炜.兰州市污水处理厂中典型抗生素的污染特征研究[J].环境科学学报,2016,36(10):3765-3773.Gao Junhong,Wang Zhaowei.Study on pollution characteristics of typical antibiotics in Lanzhou wastewater treatment plant[J].Acta Scientiae Circumstantiae,2016,36(10):3765-3773.
[13]Munir M,Wong K,Xagoraraki I,et al.Release of antibiotic resistant bacteria and genes in the effluent and biosolids of five wastewater utilities in Michigan[J].Water Research,2011,45(2):681-693.
[14]Dutta K,Lee M Y,Lai W W,et al.Removal of pharmaceuticals and organic matter from municipal wastewater using two-stage anaerobic fluidized membrane bioreactor[J].Bioresource Technology,2014,165:42-49.
[15]Xu W H,Zhang G,Li X D,et al.Occurrence and elimination of antibiotics atfour sewage treatment plants in the Pearl River Delta(PRD),south China[J].Water Research,2007,41(19):4526-4534.
[16]Alexy R,Sommer A,Lange FT,et al.Local use of antibiotics and their input and fate in a small sewage treatment plant-significance of balancing and analysis on a local scale vs nationwide scale[J].Acta Hydrochimica et Hydrobiologica,2006,34(6):587-592.
[17]Gobel A,Thomsen A,Mcardell CS,et al.Occurrence and sorption behavior of sulfonamides,macrolides,and tripethoprim in activated sludge treatment[J].Environmental Science and Technology,2005,39(11):3981-3989.
[18]Lindberg R H,Wennberg P,Johansson M I,et al.Screening of human antibiotic substances and determination of weekly mass flows in five sewage treatmentplants in Sweden[J].Environmental Science and Technology,2005,39(10):3421-3429.
[19]De Jesus Gaffney V,Cardoso V V,Cardoso E,et al.Occurrence and behaviour of pharmaceutical compounds in a Portuguese wastewater treatment plant:removal efficiency through conventional treatment processes[J].Environmental Science and Pollution Research,2017,24(17):14717-14734.
[20]Zuccato E,Castiglioni S,Bagnati R,et al.Source,occurrence and fate ofantibiotics in the Italian aquatic environment[J].Journal of Hazardous Materials,2010,179(1/2/3):1042-1048.
[21]Luo Y L,Guo W S,Ngo H H,et al.A review on the occurrence of micropollutants in the aquatic environment and their fate and removal during wastewater treatment[J].Science of the Total Environment,2014,473/474:619-641.
[22]Watkinson A J,Murby E J,Costanzo S D.Removal of antibiotics in conventional and advanced wastewater treatment:implications for environmental discharge and wastewater recycling[J].Water Research,2007,41(18):4164-4176.
[23]Batt A L,Kim S,Aga D S.Comparison of the occurrence of antibiotics in four full-scale wastewater treatment plants with varying designs and operations[J].Chemosphere,2007,68(3):428-435.
[24]Karthikkeyan K G,Meyer M T.Occurrence of antibiotics in wastewater treatment facilities in Wisconsin,USA[J].Science of the Total Environment,2006,361(1):196-207.
[25]RosalR,Rodnguez A,Perdigon-Melon JA,et al.Occurrence of emerging pollutants in urban wastewater and their removal through biological treatment followed by ozonation[J].Water Research,2010,44(2):578-588.
[26]Vieno N,Tuhkanen T,Kronberg L.Elimination of pharmaceuticals in sewage treatment plants in Finland[J].Water Research,2007,41(5):1001-1012.
[27]Kosutic K,Dolara D,Aspergera D,et al.Removal of antibiotics from a model wastewater by RO/NF membranes[J].Separation and Purification Technology,2007,53(3):244-249.
[28]Keun J C,Sang G K,Seung H K.Removal of antibiotics by coagulation and granular activated carbon filtration[J].Journal of Hazardous Materials,2007,151(1):38-43.
[29]Serrano D,Suarez S,Lema J M,et al.Removal of persistent pharmaceutical micropollutants from sewage by addition of PAC in a sequential membrance bioreactor[J].Water Research,2011,45(16):5323-5333.
[30]Huber M M,Gobel A,Joss A,et al.Oxidation of pharmaceuticals during ozonation of municipal wastewater effluents:a pilot study[J].Environmental Science and Technology,2005,39(11):4290-4299.
[31]Liu J G,Sun Q Y,Zhang C Y,et al.Removal of typical antibiotics in the advanced treatment process of productive drinking water[J].Desalination and Water Treatment,2016,57(24):11368-1391.
[32]Angela Yu-Chen L,Lin C F,Chiou J M.O3and O3/H2O2treatment of sulfonamide and macrolide antibiotics in wastewater[J].Journal of Hazardous Materials,2009,171(1/2/3):452-458.
[33]汪艳宁,卢广守.UV/Fenton法降解四环素废水的试验研究[J].天津城市建设学院学报,2012,17(4):260-263.Wang Yanning,Lu Guangshou.Experimental study on degradation of tetracycline wastewater by UV/Fenton method[J].Journal of Tianjin Urban Construction College,2012,17(4):260-263.
[34]Sahare E,Messalemr R,Cikurelh H,et al.Fate of antibiotics in activated sludge followed by ultrafiltration(CAS-UF)and in a membrane bioreactor(MBR)[J].Water Research,2011,45(16):4827-4836.
[35]Ismail K,Osman A,Wiesner M,et al.Removal of hormones and antibiotics by nanofiltration membranes[J].Journal of Membrane Science,2008,309(1/2):94-101.
[36]Sahare,David I,Gelman Y,et al.The use of RO to remove emerging micropollutants following CAS/UF or MBR treatment of municipal wastewater[J].Desalination,2011,273(1):142-147.
[37]AlturkiA A,Tadkaew N,Mcdonald J A,et al.Combining MBR and NF/RO membrane filtration for the removal of trace organics in indirect potable water reuse application[J].Journal of Membrane Science,2010,365(1/2):206-215.
[38]Dorival-Garcia N,Zafaargomei A,Navalon A,et al.Removal of quinolone antibiotics from wastewaters by sorption and biological degradation in laboratory-scale membrane bioreactors[J].Science of the Total Environment,2013,442:317-328.
[39]Radjenovic J,Petrovic M,Barcelo D.Fate and distribution of pharmaceuticals in wastewater and sewage sludge of the conventional activated sludge(CAS)and advanced membrane bioreactor(MBR)treatment[J].Water Research,2009,43(3):831-841.
[40]Xia S Q,J ia R Y,Jing D F,Xu X T.Effect of solids retention time on antibiotics removal performance and mirobial communities in an A/O-MBRprocess[J].Bioresource Technology,2012,106:36-43.
[41]陈路平,王伟杰.UV/Fenton法降解二级出水中典型抗生素的研究[J].山东工业技术,2017,16:290-291.Chen Luping,Wang Weijie.Study on degradation of typical antibiotics in secondary effluent by UV/Fenton method[J].Shandong Industrial Technology,2017,16:290-291.
[42]Alturki A A,Tadkaew N,Mcdonald J A,et al.Combining MBR and NF/RO membrane filtration for the removal of trace organics in indirect potable water reuse applications[J].Journal of Membrane Science,2010,365(1/2):206-215.
[43]Kohler C,Venditti S,Igos E,et al.Elimination of pharmaceutical residues in biologically pretreated hospital wastewater using advanced UV irradiation technology:a comparative assessment[J].Journal of Hazardous Materials,2012,239/240:70-77.
[44]Kim S D,Cho J,Kim I S,et al.Occurrence and removal of pharmaceuticals and endocrine disruptors in South Korean surface,drinking,and waste waters[J].Water Research,2007,41(5):1013-1021.
[45]周海东,黄霞,王晓琳,等.两种工艺对污水再生水中微量有机物的去除效果[J].中国环境科学,2009,29(8):816-821.Zhou Haidong,Huang Xia,Wang Xiaolin,et al.Removal of trace organic matter in sewage reclaimed water by two processes[J].China Environmental Science,2009,29(8):816-821.
[2]陈栋,王烁阳,王玉玺,等.典型内分泌干扰物在城市污水处理过程中的去除研究进展[J].青岛理工大学学报,2018,39(6):1-9.Chen Dong,Wang Shuoyang,Wang Yuxi,et al.Research progress on removal of typical endocrine disruptors in urban sewage treatment[J].Journal of Qingdao Technological University,2018,39(6):1-9.
[3]Chai Y F,Zhang Y X,Chen M X,et al.Distribution and treatment effect of antibiotics of typical WWTPs in small town of China[J].Environmental Science,2018,39(6):2724-2731.
[4]Zhao X,Wang X C,Chen Z L,et al.Microbial community structure and pharmaceuticals and personal care products removal in a membrane bioreactor seeded with aerobic granular sludge[J].Applied Microbiology and Biotechnology,2015,99(1):425-433.
[5]Li W H,Shi Y L,Gao L H,et al.Occurrence and removal of antibiotics in a municipal wastewater reclamation plant in Beijing,China[J].Chemosphere,2013,92(4):435-444.
[6]Nie Y,Qiang Z,Zhang H,et al.Fate and seasonal variation of endocrine-disrupting chemicals in a sewage treatment plant with A/A/O process[J].Separation and Purification Technology,2012,84:9-15.
[7]Matos M,Pereira M A,Parpot P,et al.Influence of tetracycline on the microbial community composition and activity of nitrifying biofilms[J].Chemosphere,2014,117:295-302.
[8]Luo Y L,Guo W S,Ngo H H,et al.A review on the occurrence of micropollutants in the aquatic environment and their fate and removal during wastewater treatment[J].Science of the Total Environment,2014,473/474:619-641.
[9]Polesel F,Andersen H R,Trapp S,et al.Removal of antibiotics in biological wastewater treatment systems-a critical assessment using the activated sludge modeling framework for xenobiotics(ASM-X)[J].Environmental Science and Technology,2016,50(19):10316-10334.
[10]Gerbersdorf S U,Cimatoribus C,Class H,et al.Anthropogenic trace compounds(ATCs)in aquatic habitats-research needs on sources,fate,detection and toxicity to ensure timely elimination strategies and risk management[J].Environment International,2015,79(3):85-105.
[11]Li B,Zhang T.Biodegradation andadsorption of antibiotics in the activated sludge process[J].Environmental Science and Technology,2010,44(9):3468-3473.
[12]高俊红,王兆炜.兰州市污水处理厂中典型抗生素的污染特征研究[J].环境科学学报,2016,36(10):3765-3773.Gao Junhong,Wang Zhaowei.Study on pollution characteristics of typical antibiotics in Lanzhou wastewater treatment plant[J].Acta Scientiae Circumstantiae,2016,36(10):3765-3773.
[13]Munir M,Wong K,Xagoraraki I,et al.Release of antibiotic resistant bacteria and genes in the effluent and biosolids of five wastewater utilities in Michigan[J].Water Research,2011,45(2):681-693.
[14]Dutta K,Lee M Y,Lai W W,et al.Removal of pharmaceuticals and organic matter from municipal wastewater using two-stage anaerobic fluidized membrane bioreactor[J].Bioresource Technology,2014,165:42-49.
[15]Xu W H,Zhang G,Li X D,et al.Occurrence and elimination of antibiotics atfour sewage treatment plants in the Pearl River Delta(PRD),south China[J].Water Research,2007,41(19):4526-4534.
[16]Alexy R,Sommer A,Lange FT,et al.Local use of antibiotics and their input and fate in a small sewage treatment plant-significance of balancing and analysis on a local scale vs nationwide scale[J].Acta Hydrochimica et Hydrobiologica,2006,34(6):587-592.
[17]Gobel A,Thomsen A,Mcardell CS,et al.Occurrence and sorption behavior of sulfonamides,macrolides,and tripethoprim in activated sludge treatment[J].Environmental Science and Technology,2005,39(11):3981-3989.
[18]Lindberg R H,Wennberg P,Johansson M I,et al.Screening of human antibiotic substances and determination of weekly mass flows in five sewage treatmentplants in Sweden[J].Environmental Science and Technology,2005,39(10):3421-3429.
[19]De Jesus Gaffney V,Cardoso V V,Cardoso E,et al.Occurrence and behaviour of pharmaceutical compounds in a Portuguese wastewater treatment plant:removal efficiency through conventional treatment processes[J].Environmental Science and Pollution Research,2017,24(17):14717-14734.
[20]Zuccato E,Castiglioni S,Bagnati R,et al.Source,occurrence and fate ofantibiotics in the Italian aquatic environment[J].Journal of Hazardous Materials,2010,179(1/2/3):1042-1048.
[21]Luo Y L,Guo W S,Ngo H H,et al.A review on the occurrence of micropollutants in the aquatic environment and their fate and removal during wastewater treatment[J].Science of the Total Environment,2014,473/474:619-641.
[22]Watkinson A J,Murby E J,Costanzo S D.Removal of antibiotics in conventional and advanced wastewater treatment:implications for environmental discharge and wastewater recycling[J].Water Research,2007,41(18):4164-4176.
[23]Batt A L,Kim S,Aga D S.Comparison of the occurrence of antibiotics in four full-scale wastewater treatment plants with varying designs and operations[J].Chemosphere,2007,68(3):428-435.
[24]Karthikkeyan K G,Meyer M T.Occurrence of antibiotics in wastewater treatment facilities in Wisconsin,USA[J].Science of the Total Environment,2006,361(1):196-207.
[25]RosalR,Rodnguez A,Perdigon-Melon JA,et al.Occurrence of emerging pollutants in urban wastewater and their removal through biological treatment followed by ozonation[J].Water Research,2010,44(2):578-588.
[26]Vieno N,Tuhkanen T,Kronberg L.Elimination of pharmaceuticals in sewage treatment plants in Finland[J].Water Research,2007,41(5):1001-1012.
[27]Kosutic K,Dolara D,Aspergera D,et al.Removal of antibiotics from a model wastewater by RO/NF membranes[J].Separation and Purification Technology,2007,53(3):244-249.
[28]Keun J C,Sang G K,Seung H K.Removal of antibiotics by coagulation and granular activated carbon filtration[J].Journal of Hazardous Materials,2007,151(1):38-43.
[29]Serrano D,Suarez S,Lema J M,et al.Removal of persistent pharmaceutical micropollutants from sewage by addition of PAC in a sequential membrance bioreactor[J].Water Research,2011,45(16):5323-5333.
[30]Huber M M,Gobel A,Joss A,et al.Oxidation of pharmaceuticals during ozonation of municipal wastewater effluents:a pilot study[J].Environmental Science and Technology,2005,39(11):4290-4299.
[31]Liu J G,Sun Q Y,Zhang C Y,et al.Removal of typical antibiotics in the advanced treatment process of productive drinking water[J].Desalination and Water Treatment,2016,57(24):11368-1391.
[32]Angela Yu-Chen L,Lin C F,Chiou J M.O3and O3/H2O2treatment of sulfonamide and macrolide antibiotics in wastewater[J].Journal of Hazardous Materials,2009,171(1/2/3):452-458.
[33]汪艳宁,卢广守.UV/Fenton法降解四环素废水的试验研究[J].天津城市建设学院学报,2012,17(4):260-263.Wang Yanning,Lu Guangshou.Experimental study on degradation of tetracycline wastewater by UV/Fenton method[J].Journal of Tianjin Urban Construction College,2012,17(4):260-263.
[34]Sahare E,Messalemr R,Cikurelh H,et al.Fate of antibiotics in activated sludge followed by ultrafiltration(CAS-UF)and in a membrane bioreactor(MBR)[J].Water Research,2011,45(16):4827-4836.
[35]Ismail K,Osman A,Wiesner M,et al.Removal of hormones and antibiotics by nanofiltration membranes[J].Journal of Membrane Science,2008,309(1/2):94-101.
[36]Sahare,David I,Gelman Y,et al.The use of RO to remove emerging micropollutants following CAS/UF or MBR treatment of municipal wastewater[J].Desalination,2011,273(1):142-147.
[37]AlturkiA A,Tadkaew N,Mcdonald J A,et al.Combining MBR and NF/RO membrane filtration for the removal of trace organics in indirect potable water reuse application[J].Journal of Membrane Science,2010,365(1/2):206-215.
[38]Dorival-Garcia N,Zafaargomei A,Navalon A,et al.Removal of quinolone antibiotics from wastewaters by sorption and biological degradation in laboratory-scale membrane bioreactors[J].Science of the Total Environment,2013,442:317-328.
[39]Radjenovic J,Petrovic M,Barcelo D.Fate and distribution of pharmaceuticals in wastewater and sewage sludge of the conventional activated sludge(CAS)and advanced membrane bioreactor(MBR)treatment[J].Water Research,2009,43(3):831-841.
[40]Xia S Q,J ia R Y,Jing D F,Xu X T.Effect of solids retention time on antibiotics removal performance and mirobial communities in an A/O-MBRprocess[J].Bioresource Technology,2012,106:36-43.
[41]陈路平,王伟杰.UV/Fenton法降解二级出水中典型抗生素的研究[J].山东工业技术,2017,16:290-291.Chen Luping,Wang Weijie.Study on degradation of typical antibiotics in secondary effluent by UV/Fenton method[J].Shandong Industrial Technology,2017,16:290-291.
[42]Alturki A A,Tadkaew N,Mcdonald J A,et al.Combining MBR and NF/RO membrane filtration for the removal of trace organics in indirect potable water reuse applications[J].Journal of Membrane Science,2010,365(1/2):206-215.
[43]Kohler C,Venditti S,Igos E,et al.Elimination of pharmaceutical residues in biologically pretreated hospital wastewater using advanced UV irradiation technology:a comparative assessment[J].Journal of Hazardous Materials,2012,239/240:70-77.
[44]Kim S D,Cho J,Kim I S,et al.Occurrence and removal of pharmaceuticals and endocrine disruptors in South Korean surface,drinking,and waste waters[J].Water Research,2007,41(5):1013-1021.
[45]周海东,黄霞,王晓琳,等.两种工艺对污水再生水中微量有机物的去除效果[J].中国环境科学,2009,29(8):816-821.Zhou Haidong,Huang Xia,Wang Xiaolin,et al.Removal of trace organic matter in sewage reclaimed water by two processes[J].China Environmental Science,2009,29(8):816-821.