磺胺甲恶唑和红霉素在模拟SAT系统去除效能及机制
发布时间：2019-06-05 17:27
【摘要】：污水回用是解决水资源短缺的有效途径,回用水质安全问题值得深入关注。抗生素作为世界上使用最为广泛的药物之一,不能在人畜体内被完全代谢,大部分以原态排泄并进入城市排水系统。抗生素结构复杂、性质稳定,在污水处理厂处理中去除率有限,国内、外环保工作者在城市污水处理厂二级出水中已检测到ng/L甚至μg/L级的抗生素存在。尽管二级处理出水中抗生素含量较低,但长期接触容易导致细菌产生耐药性,进而影响生态平衡并危及人类健康,以致于给污水处理厂二级出水回用带来不可忽视的隐患。土壤含水层处理技术(SAT)作为一种低成本、高效率的污水深度处理技术,广泛应用于污水回用工程。本论文在实验室构建了模拟SAT系统,进而研究了以磺胺甲恶唑(SMZ)和红霉素(EM)为代表的抗生素在上述系统中的去除效能,并定量分析好氧作用及其他作用对抗生素去除贡献,探求抗生素的迁移转化途径,揭示溶解性有机物(DOM)的存在对抗生素去除影响,并通过改良SAT系统的运行强化了抗生素的去除。论文建立水环境中优先控制抗生素筛选体系,通过分析典型抗生素的存在持久性、含量以及毒性并进行综合评分,筛选出对环境潜在危害最大的抗生素作为研究对象,最终确定为SMZ和EM。使用高效液相色谱检测SAT系统出水中两种抗生素浓度,发现人工合成配水中SMZ在SAT系统中去除率为87.54%,EM为92.94%。在两组土壤柱配水中加入Na N3抑制好氧微生物活性后,对比分析发现好氧生物作用相比其他作用对两种抗生素的去除贡献较大,尤其对EM。考察土壤柱不同高度对抗生素的去除,发现55.05%的SMZ的去除发生在土壤柱25~50 cm段,而土壤柱的0~25cm、50~75cm对EM的贡献最大,分别贡献了45.86%、24.27%。使用高效液相质谱联用方法分析经过SAT系统处理后出水中的抗生素的中间产物,发现SMZ有4种由N-S键断键及异恶环变化产生的降解产物,EM有6种分别由大环内酯环变化和脱去氧糖胺及克拉定糖生成的产物。为探明DOM对抗生素去除影响,研究了实际污水厂二级出水中抗生素在SAT系统的去除率,与配水中抗生素去除率相比,SMZ去除率下降到72.04%,EM的去除率则下降至64.74%。通过XAD树脂将DOM分级发现过渡亲水有机酸(TPI-A)及疏水性有机酸(HPO-A)中腐殖酸对吸附位点的争夺是导致两种抗生素去除率下降的共同原因,而EM去除率下降较大与降解EM的菌群对小分子亲水性组分(HPI)利用效果差有关,外加碳源不够,EM共代谢作用受抑制。通过对比粉煤灰与土壤对抗生素的吸附特性,发现粉煤灰对两种抗生素的吸附量均大于土壤。但粉煤灰的添加对土壤过氧化氢酶活性有抑制,综合考虑,确定土壤、粉煤灰以体积比5:1的比例、土壤柱上层25cm覆土的形式改良SAT系统,改良后的SAT系统对SMZ的去除率提高到79.16%,EM去除效率提高到68.11%,说明改良后的SAT系统对强化去除实际污水中二级出水中的SMZ的效果更好。本研究成果对于实现二级出水的高效、安全的回灌地下具有重大的理论意义和实用价值。
[Abstract]:The reuse of sewage is an effective way to solve the shortage of water resources, and the problem of recycling water quality is of great concern. As one of the most widely used drugs in the world, antibiotics cannot be fully metabolized in human and animal body, most of which are excreted in the original state and enter the urban drainage system. The structure of the antibiotic is complicated, the property is stable, the removal rate is limited in the treatment of the sewage treatment plant, and the domestic and external environmental protection workers have detected the presence of an antibiotic of ng/ L or even. mu. g/ L in the secondary effluent water of the urban sewage treatment plant. In spite of that low antibiotic content in the secondary treatment, the long-term contact lead to the drug resistance of the bacteria, thereby affecting the ecological balance and endangering the human health, so that the secondary effluent of the sewage treatment plant can not be neglected. As a kind of low-cost and high-efficiency sewage treatment technology, the soil-aquifer treatment technology (SAT) is widely used in the sewage reuse project. In this paper, the simulated SAT system was constructed in the laboratory, and the removal efficiency of antibiotics in the above-mentioned system was studied by using the antibiotics of sulfanilamide (SMZ) and erythromycin (EM), and the effect of oxygen and other action on the removal of antibiotics was quantitatively analyzed. In this paper, the effect of the presence of soluble organic matter (DOM) on the removal of antibiotics was revealed, and the removal of antibiotics was enhanced by improving the operation of the SAT system. In order to study the persistent, content and toxicity of the typical antibiotics, the antibiotic selection system was first controlled in the water environment, and the most important antibiotics were selected as the research object by analyzing the persistence, the content and the toxicity of the typical antibiotics, and finally determined to be SMZ and EM. Using high performance liquid chromatography to detect the concentration of two kinds of antibiotics in the water, the removal rate of SMZ in the synthetic water was 87.54% and the EM was 92.94%. After the addition of Na _ 3 in the two groups of soil column water to inhibit the aerobic microbial activity, the comparison and analysis showed that the effect of aerobic biological action on the removal of the two kinds of antibiotics was relatively large, especially for EM. The removal of antibiotic from different height of soil column was studied. The removal of 55.05% of SMZ was found in 25-50 cm of soil column, and the contribution of soil column 0-25 cm and 50-75 cm to EM was the largest, and the contribution to EM was 45.86% and 24.27%, respectively. The intermediate product of antibiotic in water after treatment with SAT system was analyzed by high-performance liquid-phase mass spectrometry. There are four degradation products produced by the change of N-S bond and the change of the isochal ring in SMZ. The EM has six products, respectively, which are produced by the change of macrolide rings and the removal of the glycosaminoglycans and the clavulated sugar. In order to find out the effect of DOM on the removal of antibiotics, the removal rate of antibiotics in the secondary effluent of the actual sewage plant in the SAT system was studied, and the removal rate of the SMZ was reduced to 72.04%, and the removal rate of EM decreased to 64.74%. A common cause of the reduction of the removal rate of the two kinds of antibiotics was found by the XAD resin, which found that the scramble for the adsorption sites of the humic acid in the transition hydrophilic organic acid (TPI-A) and the hydrophobic organic acid (HPO-A) was the common cause of the reduction of the removal rate of the two antibiotics, However, the degradation of EM removal was related to the poor effect of the micromolecule hydrophilic component (HPI), and the external carbon source was not enough, and the effect of EM co-metabolism was inhibited. By comparing the adsorption characteristics of fly ash and soil to antibiotics, the adsorption capacity of fly ash to both antibiotics was found to be greater than that of the soil. but the addition of the fly ash has the effect of inhibiting the activity of the catalase in the soil, comprehensively considering, determining the ratio of the volume ratio of the soil and the fly ash to the volume ratio of 5:1, improving the SAT system in the form of 25 cm soil covering the upper layer of the soil column, improving the removal rate of the modified SAT system to 79.16%, improving the EM removal efficiency to 68.11%, The results show that the modified SAT system has a better effect on strengthening the SMZ in the secondary effluent from the actual sewage. The results of this research are of great theoretical and practical value for the efficient and safe recharge of secondary effluent.
【学位授予单位】：哈尔滨工业大学
【学位级别】：硕士
【学位授予年份】：2015
【分类号】：X703
本文编号：2493698
[Abstract]:The reuse of sewage is an effective way to solve the shortage of water resources, and the problem of recycling water quality is of great concern. As one of the most widely used drugs in the world, antibiotics cannot be fully metabolized in human and animal body, most of which are excreted in the original state and enter the urban drainage system. The structure of the antibiotic is complicated, the property is stable, the removal rate is limited in the treatment of the sewage treatment plant, and the domestic and external environmental protection workers have detected the presence of an antibiotic of ng/ L or even. mu. g/ L in the secondary effluent water of the urban sewage treatment plant. In spite of that low antibiotic content in the secondary treatment, the long-term contact lead to the drug resistance of the bacteria, thereby affecting the ecological balance and endangering the human health, so that the secondary effluent of the sewage treatment plant can not be neglected. As a kind of low-cost and high-efficiency sewage treatment technology, the soil-aquifer treatment technology (SAT) is widely used in the sewage reuse project. In this paper, the simulated SAT system was constructed in the laboratory, and the removal efficiency of antibiotics in the above-mentioned system was studied by using the antibiotics of sulfanilamide (SMZ) and erythromycin (EM), and the effect of oxygen and other action on the removal of antibiotics was quantitatively analyzed. In this paper, the effect of the presence of soluble organic matter (DOM) on the removal of antibiotics was revealed, and the removal of antibiotics was enhanced by improving the operation of the SAT system. In order to study the persistent, content and toxicity of the typical antibiotics, the antibiotic selection system was first controlled in the water environment, and the most important antibiotics were selected as the research object by analyzing the persistence, the content and the toxicity of the typical antibiotics, and finally determined to be SMZ and EM. Using high performance liquid chromatography to detect the concentration of two kinds of antibiotics in the water, the removal rate of SMZ in the synthetic water was 87.54% and the EM was 92.94%. After the addition of Na _ 3 in the two groups of soil column water to inhibit the aerobic microbial activity, the comparison and analysis showed that the effect of aerobic biological action on the removal of the two kinds of antibiotics was relatively large, especially for EM. The removal of antibiotic from different height of soil column was studied. The removal of 55.05% of SMZ was found in 25-50 cm of soil column, and the contribution of soil column 0-25 cm and 50-75 cm to EM was the largest, and the contribution to EM was 45.86% and 24.27%, respectively. The intermediate product of antibiotic in water after treatment with SAT system was analyzed by high-performance liquid-phase mass spectrometry. There are four degradation products produced by the change of N-S bond and the change of the isochal ring in SMZ. The EM has six products, respectively, which are produced by the change of macrolide rings and the removal of the glycosaminoglycans and the clavulated sugar. In order to find out the effect of DOM on the removal of antibiotics, the removal rate of antibiotics in the secondary effluent of the actual sewage plant in the SAT system was studied, and the removal rate of the SMZ was reduced to 72.04%, and the removal rate of EM decreased to 64.74%. A common cause of the reduction of the removal rate of the two kinds of antibiotics was found by the XAD resin, which found that the scramble for the adsorption sites of the humic acid in the transition hydrophilic organic acid (TPI-A) and the hydrophobic organic acid (HPO-A) was the common cause of the reduction of the removal rate of the two antibiotics, However, the degradation of EM removal was related to the poor effect of the micromolecule hydrophilic component (HPI), and the external carbon source was not enough, and the effect of EM co-metabolism was inhibited. By comparing the adsorption characteristics of fly ash and soil to antibiotics, the adsorption capacity of fly ash to both antibiotics was found to be greater than that of the soil. but the addition of the fly ash has the effect of inhibiting the activity of the catalase in the soil, comprehensively considering, determining the ratio of the volume ratio of the soil and the fly ash to the volume ratio of 5:1, improving the SAT system in the form of 25 cm soil covering the upper layer of the soil column, improving the removal rate of the modified SAT system to 79.16%, improving the EM removal efficiency to 68.11%, The results show that the modified SAT system has a better effect on strengthening the SMZ in the secondary effluent from the actual sewage. The results of this research are of great theoretical and practical value for the efficient and safe recharge of secondary effluent.
【学位授予单位】：哈尔滨工业大学
【学位级别】：硕士
【学位授予年份】：2015
【分类号】：X703
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