三类抗生素在两种典型猪场废水处理工艺中的去除效果
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摘要
为了解规模化养猪场中废水处理工艺对抗生素的去除效果,选取了天津两家典型规模化猪场,采集各个处理单元出水,分析三类典型兽用抗生素(磺胺类SAs、喹诺酮类FQs和四环素类TCs)在不同处理工艺水相中的分布迁移(生猪养殖场F1工艺:原水-暂存池-固液分离后-CSTR/UASB-初沉池-A池-O池-二沉池;生猪养殖场F2工艺:原水-三级沉淀池-固液分离后-折流厌氧池-好氧曝气池-植物塘),并比较了养殖场进、出水中抗生素总承载量情况。研究结果表明:各抗生素残留浓度在不同处理单元中残留规律差异较大,F1养殖场废水共检测出10种抗生素,原水中磺胺二甲嘧啶(SMN)残留浓度最高为45.78μg·L-1,不同种类抗生素总去除率范围为-53.32%～99.33%,对于F1处理工艺,UASB单元对SAs、TCs去除效果最好,O池对FQs的去除效果较好,抗生素在进出水中总承载量分别为9 854.43 mg·d-1和1 214.49 mg·d-1;F2养殖场废水中共检测出5种抗生素,原水中恩诺沙星(ENR)残留浓度最高为8.86μg·L-1,不同种类抗生素总去除率范围为-6.95%～78.80%,其中三级沉淀池对SAs、FQs处理效果较好,植物塘对TCs去除效果较好,抗生素在进出水中总承载量分别为2 014.90 mg·d-1和1 527.96 mg·d-1。总之,F1工艺对抗生素去除效果较为明显,且厌氧、好氧处理单元对F1和F2养猪场废水中抗生素去除相对有效,因此建议猪场废水工艺中采用厌氧和好氧工艺交替处理对水相中抗生素进行去除。
To understand the antibiotic removal effect in the wastewater treatment process of large-scale swine farms, three kinds of typical veterinary antibiotics[sulfonamides(SAs), quinolones(FQs), and tetracyclines(TCs)] in the effluent of each processing unit from two typi?cal large-scale swine farms in Tianjin, China were analyzed. The distribution and total mass loading of these antibiotics were also investi?gated in the two selected farms. The results showed that the residual concentrations of the antibiotics were different in the various treatmentunits. Ten kinds of antibiotics were detected in the F1 swine farm. The highest concentration of sulfadimidine(SMN)was 45.78 μg·L-1 andthe total aqueous removal rates of antibiotics varied from-53.32% to 99.33%. The aqueous removal rates of SAs and TCs were highest inthe Up-flow Anaerobic Sludge Bed(UASB), and the aqueous removal rates of FQs were highest in the O pool. The aqueous mass loading ofinfluent and effluent in F1 was 9 854.43 mg·d-1 and 1 214.49 mg·d-1, respectively. Five kinds of antibiotics were detected in the F2 swinefarm. The highest concentration of enrofloxacin(ENR)was 8.86 μg·L-1 and the total aqueous removal rates of antibiotics varied from-6.95% to 78.80%. The aqueous removal rates of SAs and FQs were highest in the tertiary sedimentation pool, and the aqueous removalrates of TCs were highest in the plant pond. The aqueous mass loading of influent and effluent in F2 was 2 014.90 mg·d-1 and 1 527.96 mg·d-1, respectively. The F1 process could clearly remove antibiotics, and antibiotics in F1 and F2 were effectively removed in the anaerobicand oxic phases. Therefore, the alternate treatment of anaerobic and aerobic processes is recommended as the most effective way to remove antibiotics in the aqueous phase.
To understand the antibiotic removal effect in the wastewater treatment process of large-scale swine farms, three kinds of typical veterinary antibiotics[sulfonamides(SAs), quinolones(FQs), and tetracyclines(TCs)] in the effluent of each processing unit from two typi?cal large-scale swine farms in Tianjin, China were analyzed. The distribution and total mass loading of these antibiotics were also investi?gated in the two selected farms. The results showed that the residual concentrations of the antibiotics were different in the various treatmentunits. Ten kinds of antibiotics were detected in the F1 swine farm. The highest concentration of sulfadimidine(SMN)was 45.78 μg·L-1 andthe total aqueous removal rates of antibiotics varied from-53.32% to 99.33%. The aqueous removal rates of SAs and TCs were highest inthe Up-flow Anaerobic Sludge Bed(UASB), and the aqueous removal rates of FQs were highest in the O pool. The aqueous mass loading ofinfluent and effluent in F1 was 9 854.43 mg·d-1 and 1 214.49 mg·d-1, respectively. Five kinds of antibiotics were detected in the F2 swinefarm. The highest concentration of enrofloxacin(ENR)was 8.86 μg·L-1 and the total aqueous removal rates of antibiotics varied from-6.95% to 78.80%. The aqueous removal rates of SAs and FQs were highest in the tertiary sedimentation pool, and the aqueous removalrates of TCs were highest in the plant pond. The aqueous mass loading of influent and effluent in F2 was 2 014.90 mg·d-1 and 1 527.96 mg·d-1, respectively. The F1 process could clearly remove antibiotics, and antibiotics in F1 and F2 were effectively removed in the anaerobicand oxic phases. Therefore, the alternate treatment of anaerobic and aerobic processes is recommended as the most effective way to remove antibiotics in the aqueous phase.
引文
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[4]Huang X,Zheng J,Liu C,et al.Removal of antibiotics and resistance genes from swine wastewater using vertical flow constructed wetlands:Effect of hydraulic flow direction and substrate type[J].Chemical Engineering Journal,2017,308:692-699.
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[7]卫丹,万梅,刘锐,等.嘉兴市规模化养猪场沼液水质调查研究[J].环境科学,2014,35(7):2650-2657.WEI Dan,WAN Mei,LIU Rui,et al.Study on the quality of digested swinegery wastewater in large-scale farms in Jiaxing[J].Environmental Science,2014,35(7):2650-2657.
[8]Luo Y,Xu L,Rysa M,et al.Occurrence and transport of tetracycline,sulfonamide,quinolone,and macrolide antibiotics in the Haihe River basin,China[J].Environmental Science&Technology,2011,45(5):1827-1833.
[9]闾幸,余卫娟,兰亚琼,等.嘉兴市地表水中兽用抗生素的污染现状调查[J].环境科学,2013,34(9):3368-3373.LüXing,YU Wei-juan,LAN Ya-qiong,et al.A study on the veterinary antibiotics contamination in groundwater of Jiaxing[J].Environmental Science,2013,34(9):3368-3373.
[10]Kim S-C,Caelson K.Temporal and spatial trends in the occurrence of human and veterinary antibiotics in aqueous and river sediment matrices[J].Environmental Science&Technology,2007,41(1):50-57.
[11]丁佳丽,刘锐,郑炜,等.养猪废水和污泥中11种兽用抗生素的同时分析技术及其在生物降解过程的应用[J].环境科学,2015,36(10):3918-3925.DING Jia-li,LIU Rui,ZHENG Wei,et al.Method for simultaneous determination of 11 veterinary antibiotics in swine gery wastewater and sludge and its application in biological treatment[J].Environmental Science,2015,36(10):3918-3925.
[12]柴玉峰,冯玉启,张玉秀,等.猪场废水中24种抗生素同时检测方法优化[J].环境化学,2017,36(10):2147-2154.CHAI Yu-feng,FENG Yu-qi,ZHANG Yu-xiu,et al.Optimization of an analytical method for the simultaneous determinationof 24 antibiotics in swine wastewater[J].Environmental Chemistry,2017,36(10):2147-2154.
[13]靳红梅,黄红英,管永祥,等.规模化猪场废水处理过程中四环素类和磺胺类抗生素的降解特征[J].生态与农村环境学报,2016,32(6):978-985.JIN Hong-mei,HUANG Hong-ying,GUAN Yong-xiang,et al.Characteristics of degradation tetracyclines and sulfonamides during wastewater treating process in an intensive swine farm[J].Journal of Ecology and Rural Environment,2016,32(6):978-985.
[14]Zhang M,Liu Y S,Zhao J L,et al.Occurrence,fate and mass loadings of antibiotics in two swine wastewater treatment systems[J].Science of the Total Environment,2018,639:1421-1431.
[15]姜蕾,陈书怡,杨蓉.长江三角洲地区典型废水中抗生素的初步分析[J].环境化学,2008,27(3):371-374.JIANG Lei,CHEN Shu-yi,YANG Rong,et al.Occurrence of antibiotics in the aquatic environment of the Changjiang delta,China[J].Environmental Chemistry,2008,27(3):371-374.
[16]魏瑞成,葛峰,陈明,等.江苏省畜禽养殖场水环境中四环类抗生素污染研究[J].农业环境科学学报,2010,29(6):1205-1210.WEI Rui-cheng,GE Feng,CHEN Ming,et al.Pollution of tetracyclines from livestock and poultry farms in aquatic environment in Jiangsu Province,China[J].Journal of Agro-Environment Science,2010,29(6):1205-1210.
[17]Ben W,Qiang Z,Adams C,et al.Simultaneous determination of sulfonamides,tetracyclines and tiamulin in swine wastewater by solidphase extraction and liquid chromatography-mass spectrometry[J].Journal of Chromatography A,2008,1202(2):173-180.
[18]陈红,陈杖榴,曾振灵,等.鸡猪排泄物中恩诺沙星和环丙沙星含量HPLC检测方法的建立[J].中国兽医科技,2005,35(12):1004-1007.CHEN Hong,CHEN Zhang-liu,ZENG Zhen-ling,et al.Development of HPLC method for determination of enrofloxacin and ciprofloxacin levels in excrements of chicken and swine[J].Chinese Journal of Veterinary Science and Technology,2005,35(12):1004-1007.
[19]李慧.四环素类抗生素(TCs)在活性污泥处理系统中的去除行为研究[D].山东:山东农业大学,2013.LI Hui.The study of removal of tetracycline antibiotics(TCs)in the activated sludge treatment system[D].Shandong:Shandong Agricultural University,2013.
[20]Kay P,Blackwell P A,Boxall A.A lysimeter experiment to investigate the leaching of veterinary antibiotics through a clay soil and comparison with field data[J].Environmental Pollution,2005,134(2):333-341.
[21]常红,胡建英,王乐征,等.城市污水处理厂中磺胺类抗生素的调查研究[J].科学通报,2008,53(2):159-164.CHANG Hong,HU Jian-ying,WANG Le-zheng,et al.Investigation and study on sulfonylamine antibiotics in urban sewage treatment plant[J].Chinese Science Bulletin,2008,53(2):159-164.
[22]G?bel A,Mcardell C S,Joss A,et al.Fate of sulfonamides,macrolides,and trimethoprim in different wastewater treatment technologies[J].Science of the Total Environment,2007,372(2/3):361-371.
[23]Jia A,Wan Y,Xiao Y,et al.Occurrence and fate of quinolone and fluoroquinolone antibiotics in a municipal sewage treatment plant[J].Water Research,2012,46(2):387-394.
[24]Okuda T,Yamashita N,Tanaka H,et al.Development of extraction method of pharmaceuticals and their occurrences found in Japanese wastewater treatment plants[J].Environment International,2009,35(5):815-820.
[25]Li B,Zhang T.Biodegradation and adsorption of antibiotics in the activated sludge process[J].Environmental Science&Technology,2010,44(9):3468-3473.
[26]雷慧宁.规模化猪场废氷处理工艺中抗生素和重金属残留及其生态风险[D].上海:华东师范大学,2016.LEI Hui-ning.Occurrence,fate and environmental risk assessment of veterinary antibiotics and heavy metals in typical swine wastewater treatment processes,China[D].Shanghai:East China Normal University,2016.
[27]姜凌霄.鄱阳湖区典型养猪场废水抗生素污染特征及催化降解研究[D].南昌:南昌航空大学,2012.JIANG Ling-xiao.Pollution characteristics of typical antibiotics in livestock wastewater from Poyang Lake district and its photocatalytic degradation[D].Nanchang:Nanchang Hangkong University,2012.
[28]邵一如.污水处理厂中抗生素分布及影响效应研究[D].保定:河北农业大学,2013.SHAO Yi-ru.The distribution of antibiotics in wastewater treatment plant and their effects to biological treatment process[D].Baoding:Agricultural University of Hebei,2013.
[29]郭隽,张亚雷,周雪飞,等.城市污水中氟喹诺酮类抗生素药物的来源与去除研究进展[J].环境污染与防治,2016,38(2):75-80.GUO Jun,ZHANG Ya-lei,ZHOU Xue-fei,et al.Occurrence and removal of fluoroquinolones in municipal sewage:A review[J].Environmental Pollution&Control,2016,38(2):75-80.
[2]Kümmerer K.Antibiotics in the aquatic environment:A review-partⅡ[J].Chemosphere,2009,75(4):417-434.
[3]Sarmah A K,Meyer M T,Boxall A B.A global perspective on the use,sales,exposure pathways,occurrence,fate and effects of veterinary antibiotics(VAs)in the environment[J].Chemosphere,2006,65(5):725-759.
[4]Huang X,Zheng J,Liu C,et al.Removal of antibiotics and resistance genes from swine wastewater using vertical flow constructed wetlands:Effect of hydraulic flow direction and substrate type[J].Chemical Engineering Journal,2017,308:692-699.
[5]Zhao L,Dong Y H,Wang H.Residues of veterinary antibiotics in manures from feedlot livestock in eight provinces of China[J].Science of the Total Environment,2010,408(5):1069-1075.
[6]G?bel A,Thomsen A,Mcardell C S,et al.Occurrence and sorption behavior of sulfonamides,macrolides,and trimethoprim in activated sludge treatment[J].Environmental Science&Technology,2005,39(11):3981-3989.
[7]卫丹,万梅,刘锐,等.嘉兴市规模化养猪场沼液水质调查研究[J].环境科学,2014,35(7):2650-2657.WEI Dan,WAN Mei,LIU Rui,et al.Study on the quality of digested swinegery wastewater in large-scale farms in Jiaxing[J].Environmental Science,2014,35(7):2650-2657.
[8]Luo Y,Xu L,Rysa M,et al.Occurrence and transport of tetracycline,sulfonamide,quinolone,and macrolide antibiotics in the Haihe River basin,China[J].Environmental Science&Technology,2011,45(5):1827-1833.
[9]闾幸,余卫娟,兰亚琼,等.嘉兴市地表水中兽用抗生素的污染现状调查[J].环境科学,2013,34(9):3368-3373.LüXing,YU Wei-juan,LAN Ya-qiong,et al.A study on the veterinary antibiotics contamination in groundwater of Jiaxing[J].Environmental Science,2013,34(9):3368-3373.
[10]Kim S-C,Caelson K.Temporal and spatial trends in the occurrence of human and veterinary antibiotics in aqueous and river sediment matrices[J].Environmental Science&Technology,2007,41(1):50-57.
[11]丁佳丽,刘锐,郑炜,等.养猪废水和污泥中11种兽用抗生素的同时分析技术及其在生物降解过程的应用[J].环境科学,2015,36(10):3918-3925.DING Jia-li,LIU Rui,ZHENG Wei,et al.Method for simultaneous determination of 11 veterinary antibiotics in swine gery wastewater and sludge and its application in biological treatment[J].Environmental Science,2015,36(10):3918-3925.
[12]柴玉峰,冯玉启,张玉秀,等.猪场废水中24种抗生素同时检测方法优化[J].环境化学,2017,36(10):2147-2154.CHAI Yu-feng,FENG Yu-qi,ZHANG Yu-xiu,et al.Optimization of an analytical method for the simultaneous determinationof 24 antibiotics in swine wastewater[J].Environmental Chemistry,2017,36(10):2147-2154.
[13]靳红梅,黄红英,管永祥,等.规模化猪场废水处理过程中四环素类和磺胺类抗生素的降解特征[J].生态与农村环境学报,2016,32(6):978-985.JIN Hong-mei,HUANG Hong-ying,GUAN Yong-xiang,et al.Characteristics of degradation tetracyclines and sulfonamides during wastewater treating process in an intensive swine farm[J].Journal of Ecology and Rural Environment,2016,32(6):978-985.
[14]Zhang M,Liu Y S,Zhao J L,et al.Occurrence,fate and mass loadings of antibiotics in two swine wastewater treatment systems[J].Science of the Total Environment,2018,639:1421-1431.
[15]姜蕾,陈书怡,杨蓉.长江三角洲地区典型废水中抗生素的初步分析[J].环境化学,2008,27(3):371-374.JIANG Lei,CHEN Shu-yi,YANG Rong,et al.Occurrence of antibiotics in the aquatic environment of the Changjiang delta,China[J].Environmental Chemistry,2008,27(3):371-374.
[16]魏瑞成,葛峰,陈明,等.江苏省畜禽养殖场水环境中四环类抗生素污染研究[J].农业环境科学学报,2010,29(6):1205-1210.WEI Rui-cheng,GE Feng,CHEN Ming,et al.Pollution of tetracyclines from livestock and poultry farms in aquatic environment in Jiangsu Province,China[J].Journal of Agro-Environment Science,2010,29(6):1205-1210.
[17]Ben W,Qiang Z,Adams C,et al.Simultaneous determination of sulfonamides,tetracyclines and tiamulin in swine wastewater by solidphase extraction and liquid chromatography-mass spectrometry[J].Journal of Chromatography A,2008,1202(2):173-180.
[18]陈红,陈杖榴,曾振灵,等.鸡猪排泄物中恩诺沙星和环丙沙星含量HPLC检测方法的建立[J].中国兽医科技,2005,35(12):1004-1007.CHEN Hong,CHEN Zhang-liu,ZENG Zhen-ling,et al.Development of HPLC method for determination of enrofloxacin and ciprofloxacin levels in excrements of chicken and swine[J].Chinese Journal of Veterinary Science and Technology,2005,35(12):1004-1007.
[19]李慧.四环素类抗生素(TCs)在活性污泥处理系统中的去除行为研究[D].山东:山东农业大学,2013.LI Hui.The study of removal of tetracycline antibiotics(TCs)in the activated sludge treatment system[D].Shandong:Shandong Agricultural University,2013.
[20]Kay P,Blackwell P A,Boxall A.A lysimeter experiment to investigate the leaching of veterinary antibiotics through a clay soil and comparison with field data[J].Environmental Pollution,2005,134(2):333-341.
[21]常红,胡建英,王乐征,等.城市污水处理厂中磺胺类抗生素的调查研究[J].科学通报,2008,53(2):159-164.CHANG Hong,HU Jian-ying,WANG Le-zheng,et al.Investigation and study on sulfonylamine antibiotics in urban sewage treatment plant[J].Chinese Science Bulletin,2008,53(2):159-164.
[22]G?bel A,Mcardell C S,Joss A,et al.Fate of sulfonamides,macrolides,and trimethoprim in different wastewater treatment technologies[J].Science of the Total Environment,2007,372(2/3):361-371.
[23]Jia A,Wan Y,Xiao Y,et al.Occurrence and fate of quinolone and fluoroquinolone antibiotics in a municipal sewage treatment plant[J].Water Research,2012,46(2):387-394.
[24]Okuda T,Yamashita N,Tanaka H,et al.Development of extraction method of pharmaceuticals and their occurrences found in Japanese wastewater treatment plants[J].Environment International,2009,35(5):815-820.
[25]Li B,Zhang T.Biodegradation and adsorption of antibiotics in the activated sludge process[J].Environmental Science&Technology,2010,44(9):3468-3473.
[26]雷慧宁.规模化猪场废氷处理工艺中抗生素和重金属残留及其生态风险[D].上海:华东师范大学,2016.LEI Hui-ning.Occurrence,fate and environmental risk assessment of veterinary antibiotics and heavy metals in typical swine wastewater treatment processes,China[D].Shanghai:East China Normal University,2016.
[27]姜凌霄.鄱阳湖区典型养猪场废水抗生素污染特征及催化降解研究[D].南昌:南昌航空大学,2012.JIANG Ling-xiao.Pollution characteristics of typical antibiotics in livestock wastewater from Poyang Lake district and its photocatalytic degradation[D].Nanchang:Nanchang Hangkong University,2012.
[28]邵一如.污水处理厂中抗生素分布及影响效应研究[D].保定:河北农业大学,2013.SHAO Yi-ru.The distribution of antibiotics in wastewater treatment plant and their effects to biological treatment process[D].Baoding:Agricultural University of Hebei,2013.
[29]郭隽,张亚雷,周雪飞,等.城市污水中氟喹诺酮类抗生素药物的来源与去除研究进展[J].环境污染与防治,2016,38(2):75-80.GUO Jun,ZHANG Ya-lei,ZHOU Xue-fei,et al.Occurrence and removal of fluoroquinolones in municipal sewage:A review[J].Environmental Pollution&Control,2016,38(2):75-80.
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