混凝沉淀-UF工艺去除二级出水中ARGs效能研究
|
摘要
为了研究混凝沉淀-UF工艺对城市污水处理厂二级出水中ARGs (抗生素抗性基因)去除的影响,以PACl (聚合氯化铝)和PFS (聚合硫酸铁)作为混凝剂,采用q PCR(实时荧光定量聚合酶链式反应)和EEM(三维荧光光谱)等分析混凝沉淀-UF工艺对ARGs的削减及其影响因素.结果表明:①PACl、PFS投加量(分别以Al、Fe计,下同)分别为0. 85、0. 50 mmol/L时,与直接UF工艺相比,混凝沉淀-UF工艺对水中各类ARGs的去除量高2～3个数量级,其中PACl-UF工艺的效果更好,去除量为2. 51～3. 52个数量级;对水中DOC(溶解性有机碳)、富里酸类及溶解性微生物代谢产物的去除效果更好,DOC去除率由18%升至36%.②直接UF、PACl-UF、PFS-UF 3种工艺膜进、出水的线性拟合结果显示,ARGs浓度与ρ(DOC)、16S r DNA浓度均呈显著正相关.研究显示,混凝沉淀-UF工艺可以有效去除二级出水中的ARGs,且有机物、16S r DNA的去除有助于ARGs的削减.
In order to study the effect of a coagulation sedimentation-UF process on the removal of antibiotic resistance genes( ARGs) in the secondary effluent from wastewater treatment plants( WWPTs),the degree and the factors of ARGs reduction by polyaluminum chloride( PACl) and polyferric sulfate( PFS) coagulants were analyzed by real-time fluorescence quantitative polymerase chain reaction( q PCR) and three-dimensional fluorescence spectrum scanner( EEM). When the PAC1 was 0. 85 mmol/L as Al and the PFS was 0. 50 mmol/L as Fe,the removal of ARGs by the coagulation sedimentation-UF was 2-log to 3-log higher than by direct UF,and the removal efficiency of ARGs by PACl-UF was 2. 51-log to 3. 52-log. Compared to direct UF,the coagulation sedimentation-UF process had better removal of DOC( dissolved organic carbon),fulvic acid and soluble microbial metabolites,and the DOC removal rate increased from 18%to 36%. The results of the linear fitting of the membrane influent and effluent of the direct UF,PAC1-UF,and PFS-UF indicated that the ARGs had significant positive correlations with organic matter and 16 S r DNA. The study showed that the ARGs in the secondary effluent could be effectively removed by the coagulation sedimentation-UF process,and the removal of organic matter and 16 S r DNA contributed to the reduction of ARGs.
In order to study the effect of a coagulation sedimentation-UF process on the removal of antibiotic resistance genes( ARGs) in the secondary effluent from wastewater treatment plants( WWPTs),the degree and the factors of ARGs reduction by polyaluminum chloride( PACl) and polyferric sulfate( PFS) coagulants were analyzed by real-time fluorescence quantitative polymerase chain reaction( q PCR) and three-dimensional fluorescence spectrum scanner( EEM). When the PAC1 was 0. 85 mmol/L as Al and the PFS was 0. 50 mmol/L as Fe,the removal of ARGs by the coagulation sedimentation-UF was 2-log to 3-log higher than by direct UF,and the removal efficiency of ARGs by PACl-UF was 2. 51-log to 3. 52-log. Compared to direct UF,the coagulation sedimentation-UF process had better removal of DOC( dissolved organic carbon),fulvic acid and soluble microbial metabolites,and the DOC removal rate increased from 18%to 36%. The results of the linear fitting of the membrane influent and effluent of the direct UF,PAC1-UF,and PFS-UF indicated that the ARGs had significant positive correlations with organic matter and 16 S r DNA. The study showed that the ARGs in the secondary effluent could be effectively removed by the coagulation sedimentation-UF process,and the removal of organic matter and 16 S r DNA contributed to the reduction of ARGs.
引文
[1] WESTERHOFF P,YOON Y,SNYDER S,et al.Fate of endocrinedisruptor,pharmaceutical,and personal care product chemicals during simulated drinking water treatment processes[J].Environmental Science&Technology,2005,39(17):6649-6663.
[2] DAVIES J,DAVIES D.Origins and evolution of antibiotic resistance[J]. Microbiology and Molecular Biology Reviews,2010,74(3):417-433.
[3] BAQUERO F,MARTNEZ J L,CANTO'N R. Antibiotics and antibiotic resistance in water environments[J]. Current Opinion in Biotechnology,2008,19(3):260-265.
[4] ZHANG Xuxiang,ZHANG Tong,FANG H H.Antibiotic resistance genes in water environment[J]. Applied Microbiology and Biotechnology,2009,82(3):397-414.
[5] LUO Yi,MAO Daqing,RYSZ M,et al. Trends in antibiotic resistance genes occurrence in the Haihe River,China[J].Environmental Science&Technology,2010,44(19):7220-7225.
[6] AUERBACH E A,SEYFRIED E E,MCMAHON K D.Tetracycline resistance genes in activated sludge wastewater treatment plants[J].Water Research,2007,41(5):1143-1151.
[7] CHEN Hong,ZHANG Mingmei. Effects of advanced treatment systems on the removal of antibiotic resistance genes in wastewater treatment plants from Hangzhou,China[J]. Environmental Science&Technology,2013,47(15):8157-8163.
[8] GAZE W H,ZHANG Lihong,ABDOUSLAM N A,et al.Impacts of anthropogenic activity on the ecology of class 1 integrons and integron-associated genes in the environment[J]. The ISME Journal,2011,5(8):1253-1260.
[9] CZEKALSKI N,BERTHOLD T,CAUCCI S,et al.Increased levels of multiresistant bacteria and resistance genes after wastewater treatment and their dissemination into Lake Geneva,Switzerland[J].Frontiers in Microbiology,2012,3:106-112.
[10] KIM S,PARK H,CHANDRAN K.Propensity of activated sludge to amplify or attenuate tetracycline resistance genes and tetracycline resistant bacteria:a mathematical modeling approach[J].Chemosphere,2010,78(9):1071-1077.
[11] LYU S,CHEN Weiping,ZHANG Weiling,et al. Wastewater reclamation and reuse in China:opportunities and challenges[J].Journal of Environmental Sciences,2016,39:86-96.
[12] LIU Shuang,PERSSO N,KENNETH M.Situations of water reuse in China[J].Water Policy,2013,15(5):705-727.
[13] ACERO J L,BENITEZ F J,REAL F J,et al.Removal of emerging contaminants from secondary effluents by micellar-enhanced ultrafiltration[J]. Separation and Purification Technology,2017,181:123-131.
[14] BREAZEAL M V R,NOVAK J T,VIKESLAND P J,et al.Effect of wastewater colloids on membrane removal of antibiotic resistance genes[J].Water Research,2013,47(1):130-140.
[15] RIZZO L,MANAIA C,MERLIN C,et al. Urban wastewater treatment plants as hotspots for antibiotic resistant bacteria and genes spread into the environment:a review[J].Science of the Total Environment,2013,447:345-360.
[16] GAO Pin,MUNIR M,XAGORARAKI I.Correlation of tetracycline and sulfonamide antibiotics with corresponding resistance genes and resistant bacteria in a conventional municipal wastewater treatment plant[J].Science of the Total Environment,2012,421:173-183.
[17] CAI Pin,HUANG Qing,CHEN Wei,et al. Soil colloids-bound plasmid DNA:effect on transformation of E. coli and resistance to DNase I degradation[J]. Soil Biology and Biochemistry,2007,39(5):1007-1013.
[18] TRAN N,DROGUI P,BLAIS J F,et al. Phosphorus removal from spiked municipal wastewater using either electrochemical coagulation or chemical coagulation as tertiary treatment[J].Separation and Purification Technology,2012,95:16-25.
[19] WANG Daning,LIU Lu,QIU Zhigang,et al. A new adsorptionelution technique for the concentration of aquatic extracellular antibiotic resistance genes from large volumes of water[J]. Water Research,2016,92:188-198.
[20] LI Na,SHENG Guoping,LU Yongze,et al. Removal of antibiotic resistance genes from wastewater treatment plant effluent by coagulation[J].Water Research,2017,111:204-212.
[21]陆俊宇,李伟英,赵勇,等.不同预处理工艺对超滤膜运行影响的中试试验研究[J].水处理技术,2010,36(6):119-122.LU Junyu,LI Weiying,ZHAO Yong,et al. Pilot test study on the effects of different pretreatment processes on ultrafiltration membrane operation[J]. Water Treatment Technology,2010,36(6):119-122.
[22] XIAO Feng,SIMCIK M F,GULLIVER J S.Mechanisms for removal of perfluorooctane sulfonate(PFOS)and perfluorooctanoate(PFOA)from drinking water by conventional and enhanced coagulation[J].Water Research,2013,47(1):49-56.
[23] SILICHI J M,LARTIGES B S,KAYEM G J,et al. Changes in humic acid conformation during coagulation with ferric chloride:implications for drinking water treatment[J]. Water Research,2008,42(8):2111-2123.
[24] CHEN Wen,WESTERHOFF P,LEENHEER J A,et al.Fluorescence excitation-emission matrix regional integration to quantify spectra for dissolved organic matter[J]. Environmental Science&Technology,2003,37(24):5701-5710.
[25]庄耀,任洪强,耿金菊,等.混凝法去除城市生活污水中抗性基因[J].环境工程学报,2014(12):5105-5110.ZHUANG Yao,REN Hongqiang,GENG Jinju,et al. Removal of resistance genes in urban domestic sewage by coagulation method[J]. Chinese Journal of Environmental Engineering,2014(12):5105-5110.
[26]毛吉平.电解铝生产废水回用处理中混凝剂的试验研究[J].青海环境,2007,17(3):145-147.MAO Jiping. Experimental study on coagulant in wastewater treatment of electrolytic aluminum production[J]. Qinghai Environment,2007,17(3):145-147.
[27]庄耀.污水中抗生素抗性基因的深度净化技术研究[D].南京:南京大学,2014.
[28] AMY J P B.Effect of wastewater colloids on membrane removal of microconstituent antibiotic resistance genes[D]. Virginia:Virginia Polytechnic Institute and State University.
[29]李臻,高颖鸿,蔡磊,等.PAC-MBR与BPAC-UF处理微污染原水对比研究[J].水处理技术,2016,42(1):92-95.LI Zhen,GAO Yinghong,CAI Lei,et al. Comparative study on the treatment of micro-polluted raw water by PAC-MBR and BPAC-UF[J].Water Treatment Technology,2016,42(1):92-95.
[30] PENG Mingguo,LI Huajie,LI Dongong,et al. Characterization of DOM adsorption of CNTs by using excitation:emission matrix fluorescence spectroscopy and multiway analysis[J].Environmental Technology,2017,38(11):1351-1361.
[31] HADJOUDJA S,DELUCHAT V,BAUDU M. Cell surface characterisation of microcystis aeruginosa and chlorella vulgaris[J].Journal of Colloid and Interface Science,2010,342(2):293-299.
[32] LIU Shanshan,QU Hongmei,YANG Dong,et al. Chlorine disinfection increases both intracellular and extracellular antibiotic resistance genes in a full-scale wastewater treatment plant[J].Water Research,2018,136:131-136.
[2] DAVIES J,DAVIES D.Origins and evolution of antibiotic resistance[J]. Microbiology and Molecular Biology Reviews,2010,74(3):417-433.
[3] BAQUERO F,MARTNEZ J L,CANTO'N R. Antibiotics and antibiotic resistance in water environments[J]. Current Opinion in Biotechnology,2008,19(3):260-265.
[4] ZHANG Xuxiang,ZHANG Tong,FANG H H.Antibiotic resistance genes in water environment[J]. Applied Microbiology and Biotechnology,2009,82(3):397-414.
[5] LUO Yi,MAO Daqing,RYSZ M,et al. Trends in antibiotic resistance genes occurrence in the Haihe River,China[J].Environmental Science&Technology,2010,44(19):7220-7225.
[6] AUERBACH E A,SEYFRIED E E,MCMAHON K D.Tetracycline resistance genes in activated sludge wastewater treatment plants[J].Water Research,2007,41(5):1143-1151.
[7] CHEN Hong,ZHANG Mingmei. Effects of advanced treatment systems on the removal of antibiotic resistance genes in wastewater treatment plants from Hangzhou,China[J]. Environmental Science&Technology,2013,47(15):8157-8163.
[8] GAZE W H,ZHANG Lihong,ABDOUSLAM N A,et al.Impacts of anthropogenic activity on the ecology of class 1 integrons and integron-associated genes in the environment[J]. The ISME Journal,2011,5(8):1253-1260.
[9] CZEKALSKI N,BERTHOLD T,CAUCCI S,et al.Increased levels of multiresistant bacteria and resistance genes after wastewater treatment and their dissemination into Lake Geneva,Switzerland[J].Frontiers in Microbiology,2012,3:106-112.
[10] KIM S,PARK H,CHANDRAN K.Propensity of activated sludge to amplify or attenuate tetracycline resistance genes and tetracycline resistant bacteria:a mathematical modeling approach[J].Chemosphere,2010,78(9):1071-1077.
[11] LYU S,CHEN Weiping,ZHANG Weiling,et al. Wastewater reclamation and reuse in China:opportunities and challenges[J].Journal of Environmental Sciences,2016,39:86-96.
[12] LIU Shuang,PERSSO N,KENNETH M.Situations of water reuse in China[J].Water Policy,2013,15(5):705-727.
[13] ACERO J L,BENITEZ F J,REAL F J,et al.Removal of emerging contaminants from secondary effluents by micellar-enhanced ultrafiltration[J]. Separation and Purification Technology,2017,181:123-131.
[14] BREAZEAL M V R,NOVAK J T,VIKESLAND P J,et al.Effect of wastewater colloids on membrane removal of antibiotic resistance genes[J].Water Research,2013,47(1):130-140.
[15] RIZZO L,MANAIA C,MERLIN C,et al. Urban wastewater treatment plants as hotspots for antibiotic resistant bacteria and genes spread into the environment:a review[J].Science of the Total Environment,2013,447:345-360.
[16] GAO Pin,MUNIR M,XAGORARAKI I.Correlation of tetracycline and sulfonamide antibiotics with corresponding resistance genes and resistant bacteria in a conventional municipal wastewater treatment plant[J].Science of the Total Environment,2012,421:173-183.
[17] CAI Pin,HUANG Qing,CHEN Wei,et al. Soil colloids-bound plasmid DNA:effect on transformation of E. coli and resistance to DNase I degradation[J]. Soil Biology and Biochemistry,2007,39(5):1007-1013.
[18] TRAN N,DROGUI P,BLAIS J F,et al. Phosphorus removal from spiked municipal wastewater using either electrochemical coagulation or chemical coagulation as tertiary treatment[J].Separation and Purification Technology,2012,95:16-25.
[19] WANG Daning,LIU Lu,QIU Zhigang,et al. A new adsorptionelution technique for the concentration of aquatic extracellular antibiotic resistance genes from large volumes of water[J]. Water Research,2016,92:188-198.
[20] LI Na,SHENG Guoping,LU Yongze,et al. Removal of antibiotic resistance genes from wastewater treatment plant effluent by coagulation[J].Water Research,2017,111:204-212.
[21]陆俊宇,李伟英,赵勇,等.不同预处理工艺对超滤膜运行影响的中试试验研究[J].水处理技术,2010,36(6):119-122.LU Junyu,LI Weiying,ZHAO Yong,et al. Pilot test study on the effects of different pretreatment processes on ultrafiltration membrane operation[J]. Water Treatment Technology,2010,36(6):119-122.
[22] XIAO Feng,SIMCIK M F,GULLIVER J S.Mechanisms for removal of perfluorooctane sulfonate(PFOS)and perfluorooctanoate(PFOA)from drinking water by conventional and enhanced coagulation[J].Water Research,2013,47(1):49-56.
[23] SILICHI J M,LARTIGES B S,KAYEM G J,et al. Changes in humic acid conformation during coagulation with ferric chloride:implications for drinking water treatment[J]. Water Research,2008,42(8):2111-2123.
[24] CHEN Wen,WESTERHOFF P,LEENHEER J A,et al.Fluorescence excitation-emission matrix regional integration to quantify spectra for dissolved organic matter[J]. Environmental Science&Technology,2003,37(24):5701-5710.
[25]庄耀,任洪强,耿金菊,等.混凝法去除城市生活污水中抗性基因[J].环境工程学报,2014(12):5105-5110.ZHUANG Yao,REN Hongqiang,GENG Jinju,et al. Removal of resistance genes in urban domestic sewage by coagulation method[J]. Chinese Journal of Environmental Engineering,2014(12):5105-5110.
[26]毛吉平.电解铝生产废水回用处理中混凝剂的试验研究[J].青海环境,2007,17(3):145-147.MAO Jiping. Experimental study on coagulant in wastewater treatment of electrolytic aluminum production[J]. Qinghai Environment,2007,17(3):145-147.
[27]庄耀.污水中抗生素抗性基因的深度净化技术研究[D].南京:南京大学,2014.
[28] AMY J P B.Effect of wastewater colloids on membrane removal of microconstituent antibiotic resistance genes[D]. Virginia:Virginia Polytechnic Institute and State University.
[29]李臻,高颖鸿,蔡磊,等.PAC-MBR与BPAC-UF处理微污染原水对比研究[J].水处理技术,2016,42(1):92-95.LI Zhen,GAO Yinghong,CAI Lei,et al. Comparative study on the treatment of micro-polluted raw water by PAC-MBR and BPAC-UF[J].Water Treatment Technology,2016,42(1):92-95.
[30] PENG Mingguo,LI Huajie,LI Dongong,et al. Characterization of DOM adsorption of CNTs by using excitation:emission matrix fluorescence spectroscopy and multiway analysis[J].Environmental Technology,2017,38(11):1351-1361.
[31] HADJOUDJA S,DELUCHAT V,BAUDU M. Cell surface characterisation of microcystis aeruginosa and chlorella vulgaris[J].Journal of Colloid and Interface Science,2010,342(2):293-299.
[32] LIU Shanshan,QU Hongmei,YANG Dong,et al. Chlorine disinfection increases both intracellular and extracellular antibiotic resistance genes in a full-scale wastewater treatment plant[J].Water Research,2018,136:131-136.