人工湿地对14种常用抗生素的去除效果及影响因素研究
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摘要
抗生素主要用于预防治疗人体和动物体疾病，也常作为生长促进剂添加于动物饲料中。由于抗生素的大量使用和滥用，导致病原菌对抗生素产生耐药性，其耐药速度和耐药水平呈逐年上升趋势，已对全球性环境问题构成威胁。为了改善饮用水水质和保护人群健康，提供一种经济高效去除抗生素的生物处理工艺已成为亟待解决的问题。人工湿地在处理药物和个人护理品（PPCPs）及投资运行管理方面相对于其它传统污水处理工艺具有不可比拟的优势，但对利用人工湿地去除生活污水和污水厂尾水中抗生素，以及抗生素去除效果和影响因素的研究在国内外并不多见，可供参考的抗生素去除机理、关键的设计参数等也不多。
本研究基于试验小试与野外中试、生活污水与污水厂尾水的差异性特点，研究了人工湿地对污水中抗生素的去除效果和影响因素。通过12种构型模拟人工湿地（试验小试）对生活污水中14种抗生素（磺胺类：磺胺嘧啶、磺胺吡啶、磺胺醋酰、磺胺甲噁唑、磺胺二甲嘧啶和甲氧苄啶；喹诺酮类：诺氟沙星、环丙沙星、洛美沙星和氧氟沙星；四环素类：四环素和氧四环素；大环内酯类：脱水红霉素和罗红霉素）的去除效果进行了研究，并通过正交试验分析确定了4类抗生素去除效果的主要影响因素及其影响显著性；同时研究了垂直-水平潜流组合湿地和自然曝气生物滤床（野外中试）对污水厂尾水中14种抗生素的去除效果和影响因素，以及这两种工艺处理效果间的比较。
本研究得出以下结论：
（1）试验小试对生活污水中抗生素的去除效果和影响因素
本试验选取4种工艺（下行垂直流、上行垂直流、表面流、水平潜流）、3种基质（火山石、砾石、沸石）、3种植物（再力花、花叶芦竹、无植物）、3种水力负荷（0.125、0.25、0.5m/d）构建12种构型模拟人工湿地，对生活污水中抗生素的去除效果和影响因素进行研究，结果表明：
即使在高进水浓度的条件下，不同构型的模拟湿地均能很好的去除生活污水中磺胺类、喹诺酮类、四环素类和大环内酯类。正交试验结果表明，工艺、基质和水力负荷3种因素对磺胺类的去除效率均有显著性影响（P＜0.05），但其在任一因素各水平下的去除效率均无显著性差异（P＞0.05），而工艺、基质、植物和水力负荷4种因素对喹诺酮类、四环素类和大环内酯类的去除效率均无显著性影响（P＞0.05），可见不同构型模拟湿地对这4类抗生素均有很好的去除效果，人工湿地是一种能够经济高效去除生活污水中多种抗生素的生物处理工艺。
（2）野外中试对污水厂尾水中抗生素的去除效果和影响因素
为了提高去除负荷、节约占地面积，采用由下行垂直流和水平潜流串联构成的垂直流-水平潜流组合湿地，以及由多种填料（生物陶粒、高炉渣、砾石）组成的自然曝气生物滤床两种工艺对污水厂尾水中抗生素的去除效果和影响因素进行研究，并对两种工艺的去除效果进行比较，结果显示：
组合湿地和生物滤床均能有效去除污水厂尾水中喹诺酮类、大环内酯类和四环素类抗生素，且有植物的湿地系统比无植物的滤床系统处理效果好，说明占地面积小水力负荷高的人工湿地工艺可以经济高效去除污水厂尾水中多种抗生素。此外，水力负荷对抗生素去除效果有一定的影响，组合湿地和生物滤床的适宜水力负荷分别为1.0~1.5m/d和4.8~6.4m/d。
结合试验小试和野外中试的讨论结果，总结抗生素可能的去除途径为：喹诺酮类主要通过吸附和光降解而去除，吸附和水解是四环素类的主要去除途径，而磺胺类和大环内酯类的去除则是多种途径共同作用的结果，其中植物的存在有利于大环内酯类的去除。
以上的研究结果表明采用人工湿地对生活污水中磺胺类、喹诺酮类、四环素类和大环内酯类的处理均能取得理想的去除效果，同时人工湿地对污水厂尾水中喹诺酮类、四环素类和大环内酯类均有较好的去处效果，研究所得出的抗生素的去除效果、影响因素以及人工湿地优化设计参数和可能的去除途径可作为以后利用人工湿地处理污水中抗生素的应用参考依据。
Antibiotics are mainly applied in the prevention and treatment of humans and animals’diseases, and are used as a promoter in animal feeds as well. The development and proliferationof antibiotic resistence in enviromental microorganisms is a major public health concern aroundthe world. For the sake of improve the drinking water quality and prove the health of people, weneed a economical and efficient biological treatment technology to solve the problem.Cconstructed wetland (CW) has unparalleled advantages relative to the traditional sewagetreatment process in pharmaceuticals and personal care products (PPCPs) removal andinvestment, operational management, but the research about that using CW for removal ofantibiotics in domestic sewage and sewage plant effluent and the impact factors which canimpact the antibiotic removal are rare. In addition, the removal mechanism of reference and thekey design parameters are rare, too.
This paper has researched the benefit and discipline of antibiotics removal and impactfactors of CW in the pilot test and field test, domestic sewage and sewage plant effluent. We hasstudied the removal of14antibiotics (sulfonamides: sulfadizine, sulfapyridine, sulfacetamide,sulfamethazine, sulfamethoxazole, trimethoprim; quinolones: norfloxacin, ciprofloxacin,lomefloxacin, ofloxacin; tetracyclines: oxytetracycline, tetracycline; macrolides: roxithromycin,erythromycin) in domestic sewage by12kinds of configuration simulation constructed wetlands(SCWs, pilot test), and determined the main factors and their significant by the orthogonal testwhich concluded that four classes antibiotics removal effect; Meanwhile, we has studied theremoval and impact factors of14antibiotics in sewage plant effluent by the vertical-horizontalsubsurface-flow complex constructed wetland and natural biological aerated filter (field test),and compared the removal of the two processes.
Analyses of the conclusions of the study are as follows:
(1) The removal and impact factors of antibiotics in domestic sewage by pilot test
We has studied the removal and impact factors of antibiotics in domestic sewage by12kinds of configuration simulation constructed wetland which consist of four processes (verticalsubsurface-flow CW (VFCW), upward vertical subsurface-flow CW (UVFCW), surface flowCW (SFCW), horizontal subsurface-flow CW (HFCW)), three substrates (vesuvianite, gravel, zeolite), three plants (Thalia dealbata, Arundo donax var. versicolor, unplant), three hydraulicloading rate (HLR,0.125,0.25,0.5m/d), the results shows that:
Although the concentration of some antibiotics are very high,12kinds of configurationSCWs have high removal efficiencies for sulfonamides, quinolones, tetracyclines and macrolides.The process, substrate and HLR have significant effect on the removal of sulfonamides in SCW,whose shuiping have no significant difference (P>0.05), and the process, substrate, plant andHLR have no significant effect on the removal of quinolones, tetracyclines, macrolides in SCW(P <0.05), which mean these antibiotics could be removed effectively by SCW.
(2) The removal and impact factors of antibiotics in domestic sewage by field test
For the sake of enhance the removal load and save the floor space, we has studied theremoval and impact factors in the vertical-horizontal subsurface-flow complex constructedwetland (CCW) which consist of VFCW and HFCW in series, and the natural biological aeratedfilter (BAF) with Bio-ceramic, blast furnace slag and gravel, to remove the antibiotics. Theremoval efficiency was compared, and the results shows that:
Quinolones, tetracyclines and macrolides could be eliminated effectively by CCW and BAF,and the removal of antibiotics by planted CCW system is more effective than the unplanted BAFsystem, which mean that CWs with limited area and high HLR could remove antibiotics insewage plant effluent. The treatment of antibiotics could be affected by the HLR, and the optimalHLR for the removal of antibiotics in the CCW and BAF were1.0~1.5m/d and4.8~6.4m/d,respectively.
The results about pilot test and field test also shows that, adsorption and photodegradationappears to be the most important pathways for quinolones; Tetracyclines removed by means ofadsorption processes and hydrolysis; The elimination of sulfonamides and macrolides could bethe combined action of several pathways.
The above results shows that: The CW can be used to deal with the sulfonamides,quinolones, tetracyclines and macrolides in domestic sewage, and the effluent of sulfonamidesand tetracyclines can reach the level of tertiary sewage treatment process. And the CW also canbe used to deal with the quinolones, tetracyclines and macrolides in sewage plant effluent. Theremoval efficiencies of antibiotics, the impact factors, the key design parameters of CW and thepossible elimination pathways all can be used in the CW system to deal with the antibiotics treatment in the future.
本研究基于试验小试与野外中试、生活污水与污水厂尾水的差异性特点，研究了人工湿地对污水中抗生素的去除效果和影响因素。通过12种构型模拟人工湿地（试验小试）对生活污水中14种抗生素（磺胺类：磺胺嘧啶、磺胺吡啶、磺胺醋酰、磺胺甲噁唑、磺胺二甲嘧啶和甲氧苄啶；喹诺酮类：诺氟沙星、环丙沙星、洛美沙星和氧氟沙星；四环素类：四环素和氧四环素；大环内酯类：脱水红霉素和罗红霉素）的去除效果进行了研究，并通过正交试验分析确定了4类抗生素去除效果的主要影响因素及其影响显著性；同时研究了垂直-水平潜流组合湿地和自然曝气生物滤床（野外中试）对污水厂尾水中14种抗生素的去除效果和影响因素，以及这两种工艺处理效果间的比较。
本研究得出以下结论：
（1）试验小试对生活污水中抗生素的去除效果和影响因素
本试验选取4种工艺（下行垂直流、上行垂直流、表面流、水平潜流）、3种基质（火山石、砾石、沸石）、3种植物（再力花、花叶芦竹、无植物）、3种水力负荷（0.125、0.25、0.5m/d）构建12种构型模拟人工湿地，对生活污水中抗生素的去除效果和影响因素进行研究，结果表明：
即使在高进水浓度的条件下，不同构型的模拟湿地均能很好的去除生活污水中磺胺类、喹诺酮类、四环素类和大环内酯类。正交试验结果表明，工艺、基质和水力负荷3种因素对磺胺类的去除效率均有显著性影响（P＜0.05），但其在任一因素各水平下的去除效率均无显著性差异（P＞0.05），而工艺、基质、植物和水力负荷4种因素对喹诺酮类、四环素类和大环内酯类的去除效率均无显著性影响（P＞0.05），可见不同构型模拟湿地对这4类抗生素均有很好的去除效果，人工湿地是一种能够经济高效去除生活污水中多种抗生素的生物处理工艺。
（2）野外中试对污水厂尾水中抗生素的去除效果和影响因素
为了提高去除负荷、节约占地面积，采用由下行垂直流和水平潜流串联构成的垂直流-水平潜流组合湿地，以及由多种填料（生物陶粒、高炉渣、砾石）组成的自然曝气生物滤床两种工艺对污水厂尾水中抗生素的去除效果和影响因素进行研究，并对两种工艺的去除效果进行比较，结果显示：
组合湿地和生物滤床均能有效去除污水厂尾水中喹诺酮类、大环内酯类和四环素类抗生素，且有植物的湿地系统比无植物的滤床系统处理效果好，说明占地面积小水力负荷高的人工湿地工艺可以经济高效去除污水厂尾水中多种抗生素。此外，水力负荷对抗生素去除效果有一定的影响，组合湿地和生物滤床的适宜水力负荷分别为1.0~1.5m/d和4.8~6.4m/d。
结合试验小试和野外中试的讨论结果，总结抗生素可能的去除途径为：喹诺酮类主要通过吸附和光降解而去除，吸附和水解是四环素类的主要去除途径，而磺胺类和大环内酯类的去除则是多种途径共同作用的结果，其中植物的存在有利于大环内酯类的去除。
以上的研究结果表明采用人工湿地对生活污水中磺胺类、喹诺酮类、四环素类和大环内酯类的处理均能取得理想的去除效果，同时人工湿地对污水厂尾水中喹诺酮类、四环素类和大环内酯类均有较好的去处效果，研究所得出的抗生素的去除效果、影响因素以及人工湿地优化设计参数和可能的去除途径可作为以后利用人工湿地处理污水中抗生素的应用参考依据。
Antibiotics are mainly applied in the prevention and treatment of humans and animals’diseases, and are used as a promoter in animal feeds as well. The development and proliferationof antibiotic resistence in enviromental microorganisms is a major public health concern aroundthe world. For the sake of improve the drinking water quality and prove the health of people, weneed a economical and efficient biological treatment technology to solve the problem.Cconstructed wetland (CW) has unparalleled advantages relative to the traditional sewagetreatment process in pharmaceuticals and personal care products (PPCPs) removal andinvestment, operational management, but the research about that using CW for removal ofantibiotics in domestic sewage and sewage plant effluent and the impact factors which canimpact the antibiotic removal are rare. In addition, the removal mechanism of reference and thekey design parameters are rare, too.
This paper has researched the benefit and discipline of antibiotics removal and impactfactors of CW in the pilot test and field test, domestic sewage and sewage plant effluent. We hasstudied the removal of14antibiotics (sulfonamides: sulfadizine, sulfapyridine, sulfacetamide,sulfamethazine, sulfamethoxazole, trimethoprim; quinolones: norfloxacin, ciprofloxacin,lomefloxacin, ofloxacin; tetracyclines: oxytetracycline, tetracycline; macrolides: roxithromycin,erythromycin) in domestic sewage by12kinds of configuration simulation constructed wetlands(SCWs, pilot test), and determined the main factors and their significant by the orthogonal testwhich concluded that four classes antibiotics removal effect; Meanwhile, we has studied theremoval and impact factors of14antibiotics in sewage plant effluent by the vertical-horizontalsubsurface-flow complex constructed wetland and natural biological aerated filter (field test),and compared the removal of the two processes.
Analyses of the conclusions of the study are as follows:
(1) The removal and impact factors of antibiotics in domestic sewage by pilot test
We has studied the removal and impact factors of antibiotics in domestic sewage by12kinds of configuration simulation constructed wetland which consist of four processes (verticalsubsurface-flow CW (VFCW), upward vertical subsurface-flow CW (UVFCW), surface flowCW (SFCW), horizontal subsurface-flow CW (HFCW)), three substrates (vesuvianite, gravel, zeolite), three plants (Thalia dealbata, Arundo donax var. versicolor, unplant), three hydraulicloading rate (HLR,0.125,0.25,0.5m/d), the results shows that:
Although the concentration of some antibiotics are very high,12kinds of configurationSCWs have high removal efficiencies for sulfonamides, quinolones, tetracyclines and macrolides.The process, substrate and HLR have significant effect on the removal of sulfonamides in SCW,whose shuiping have no significant difference (P>0.05), and the process, substrate, plant andHLR have no significant effect on the removal of quinolones, tetracyclines, macrolides in SCW(P <0.05), which mean these antibiotics could be removed effectively by SCW.
(2) The removal and impact factors of antibiotics in domestic sewage by field test
For the sake of enhance the removal load and save the floor space, we has studied theremoval and impact factors in the vertical-horizontal subsurface-flow complex constructedwetland (CCW) which consist of VFCW and HFCW in series, and the natural biological aeratedfilter (BAF) with Bio-ceramic, blast furnace slag and gravel, to remove the antibiotics. Theremoval efficiency was compared, and the results shows that:
Quinolones, tetracyclines and macrolides could be eliminated effectively by CCW and BAF,and the removal of antibiotics by planted CCW system is more effective than the unplanted BAFsystem, which mean that CWs with limited area and high HLR could remove antibiotics insewage plant effluent. The treatment of antibiotics could be affected by the HLR, and the optimalHLR for the removal of antibiotics in the CCW and BAF were1.0~1.5m/d and4.8~6.4m/d,respectively.
The results about pilot test and field test also shows that, adsorption and photodegradationappears to be the most important pathways for quinolones; Tetracyclines removed by means ofadsorption processes and hydrolysis; The elimination of sulfonamides and macrolides could bethe combined action of several pathways.
The above results shows that: The CW can be used to deal with the sulfonamides,quinolones, tetracyclines and macrolides in domestic sewage, and the effluent of sulfonamidesand tetracyclines can reach the level of tertiary sewage treatment process. And the CW also canbe used to deal with the quinolones, tetracyclines and macrolides in sewage plant effluent. Theremoval efficiencies of antibiotics, the impact factors, the key design parameters of CW and thepossible elimination pathways all can be used in the CW system to deal with the antibiotics treatment in the future.
引文
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