磺胺甲惡唑和紅霉素在模擬SAT系統(tǒng)去除效能及機制
發(fā)布時間：2019-06-05 17:27
【摘要】：污水回用是解決水資源短缺的有效途徑,回用水質(zhì)安全問題值得深入關注�？股刈鳛槭澜缟鲜褂米顬閺V泛的藥物之一,不能在人畜體內(nèi)被完全代謝,大部分以原態(tài)排泄并進入城市排水系統(tǒng)�？股亟Y構復雜、性質(zhì)穩(wěn)定,在污水處理廠處理中去除率有限,國內(nèi)、外環(huán)保工作者在城市污水處理廠二級出水中已檢測到ng/L甚至μg/L級的抗生素存在。盡管二級處理出水中抗生素含量較低,但長期接觸容易導致細菌產(chǎn)生耐藥性,進而影響生態(tài)平衡并危及人類健康,以致于給污水處理廠二級出水回用帶來不可忽視的隱患。土壤含水層處理技術(SAT)作為一種低成本、高效率的污水深度處理技術,廣泛應用于污水回用工程。本論文在實驗室構建了模擬SAT系統(tǒng),進而研究了以磺胺甲惡唑(SMZ)和紅霉素(EM)為代表的抗生素在上述系統(tǒng)中的去除效能,并定量分析好氧作用及其他作用對抗生素去除貢獻,探求抗生素的遷移轉(zhuǎn)化途徑,揭示溶解性有機物(DOM)的存在對抗生素去除影響,并通過改良SAT系統(tǒng)的運行強化了抗生素的去除。論文建立水環(huán)境中優(yōu)先控制抗生素篩選體系,通過分析典型抗生素的存在持久性、含量以及毒性并進行綜合評分,篩選出對環(huán)境潛在危害最大的抗生素作為研究對象,最終確定為SMZ和EM。使用高效液相色譜檢測SAT系統(tǒng)出水中兩種抗生素濃度,發(fā)現(xiàn)人工合成配水中SMZ在SAT系統(tǒng)中去除率為87.54%,EM為92.94%。在兩組土壤柱配水中加入Na N3抑制好氧微生物活性后,對比分析發(fā)現(xiàn)好氧生物作用相比其他作用對兩種抗生素的去除貢獻較大,尤其對EM�？疾焱寥乐煌叨葘股氐娜コ�,發(fā)現(xiàn)55.05%的SMZ的去除發(fā)生在土壤柱25~50 cm段,而土壤柱的0~25cm、50~75cm對EM的貢獻最大,分別貢獻了45.86%、24.27%。使用高效液相質(zhì)譜聯(lián)用方法分析經(jīng)過SAT系統(tǒng)處理后出水中的抗生素的中間產(chǎn)物,發(fā)現(xiàn)SMZ有4種由N-S鍵斷鍵及異惡環(huán)變化產(chǎn)生的降解產(chǎn)物,EM有6種分別由大環(huán)內(nèi)酯環(huán)變化和脫去氧糖胺及克拉定糖生成的產(chǎn)物。為探明DOM對抗生素去除影響,研究了實際污水廠二級出水中抗生素在SAT系統(tǒng)的去除率,與配水中抗生素去除率相比,SMZ去除率下降到72.04%,EM的去除率則下降至64.74%。通過XAD樹脂將DOM分級發(fā)現(xiàn)過渡親水有機酸(TPI-A)及疏水性有機酸(HPO-A)中腐殖酸對吸附位點的爭奪是導致兩種抗生素去除率下降的共同原因,而EM去除率下降較大與降解EM的菌群對小分子親水性組分(HPI)利用效果差有關,外加碳源不夠,EM共代謝作用受抑制。通過對比粉煤灰與土壤對抗生素的吸附特性,發(fā)現(xiàn)粉煤灰對兩種抗生素的吸附量均大于土壤。但粉煤灰的添加對土壤過氧化氫酶活性有抑制,綜合考慮,確定土壤、粉煤灰以體積比5:1的比例、土壤柱上層25cm覆土的形式改良SAT系統(tǒng),改良后的SAT系統(tǒng)對SMZ的去除率提高到79.16%,EM去除效率提高到68.11%,說明改良后的SAT系統(tǒng)對強化去除實際污水中二級出水中的SMZ的效果更好。本研究成果對于實現(xiàn)二級出水的高效、安全的回灌地下具有重大的理論意義和實用價值。
[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.
【學位授予單位】：哈爾濱工業(yè)大學
【學位級別】：碩士
【學位授予年份】：2015
【分類號】：X703
本文編號：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.
【學位授予單位】：哈爾濱工業(yè)大學
【學位級別】：碩士
【學位授予年份】：2015
【分類號】：X703
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