本文選題：抗生素　切入點：阿莫西林　出處：《哈爾濱工業(yè)大學(xué)》2015年碩士論文

【摘要】：抗生素廣泛用于治療人類和動物疾病,以及作為飼料添加劑促進(jìn)動物的生長。然而,由于其對水生生態(tài)和人類健康的潛在不利影響,出現(xiàn)在水體等自然環(huán)境中的抗生素受到特別的關(guān)注。由于抗生素具有抗菌性及生物毒性,傳統(tǒng)的生物水處理方法并不能有效的去除環(huán)境中的抗生素。因此,有必要開發(fā)高效的處理技術(shù),去除水體中的抗生素,減少抗生素對環(huán)境的影響。本文選取阿莫西林(AMO)廢水進(jìn)行研究,采用電化學(xué)氧化法,臭氧氧化法和電化學(xué)聯(lián)合臭氧氧化對其處理,并分析了臭氧氧化和電化學(xué)聯(lián)合臭氧氧化過程的作用效能及機(jī)理。在三種方法中,電化學(xué)聯(lián)合臭氧氧化是對AMO降解最有效的技術(shù)。電化學(xué)作用6分鐘后只有37%的AMO去除率,而在5分鐘和4分鐘內(nèi),AMO可以分別被臭氧和電化學(xué)聯(lián)合臭氧過程完全處理。同時,在礦化度實驗中,用電化學(xué)聯(lián)合臭氧氧化處理60分鐘后,總有機(jī)碳礦化度達(dá)到67.8%。相比較而言,使用臭氧氧化和電化學(xué)法處理,分別只得到47.3%和3.1%的礦化度。結(jié)果發(fā)現(xiàn),電化學(xué)聯(lián)合臭氧的氧化過程中羥基自由基的產(chǎn)量和O3的利用率均得到了提高。為了更加經(jīng)濟(jì)有效地控制電化學(xué)聯(lián)合臭氧處理阿莫西林過程,本文系統(tǒng)的研究了電化學(xué)聯(lián)合臭氧處理阿莫西林過程中重要的操作參數(shù),如臭氧濃度,電流,p H等對處理效能的影響。研究表明,在電化學(xué)聯(lián)合臭氧氧化過程增加曝氣中臭氧的濃度會增加阿莫西林的降解及TOC礦化度。電流從100毫安增加到300毫安時,阿莫西林的降解和TOC礦化隨著所施加電流的增加而變大。然而,進(jìn)一步增加電流至400毫安時,阿莫西林降解和TOC礦化并未提高甚至出現(xiàn)了一定的下降。本研究發(fā)現(xiàn),p H值對于AMO降解和TOC礦化起重要作用,它不僅影響水溶液中臭氧的分解和羥基自由基的產(chǎn)量,而且還影響到AMO的存在形式。此外,本研究還開展了電化學(xué)聯(lián)合臭氧降解AMO中,電化學(xué)引入對該系統(tǒng)的影響機(jī)理。結(jié)果發(fā)現(xiàn)電化學(xué)引入后確實促進(jìn)了羥基自由基的產(chǎn)生,并且提高了O3的利用率。因此,電化學(xué)聯(lián)合臭氧氧化過程相對于臭氧氧化能夠更經(jīng)濟(jì)和更有效的降解AMO。最后,開展了AMO降解途徑的研究。采用UPLC-MS/MS技術(shù)鑒定了電化學(xué)聯(lián)合臭氧和臭氧單獨氧化處理的中間產(chǎn)物。在電化學(xué)聯(lián)合臭氧氧化中發(fā)現(xiàn)了15種不同質(zhì)荷比的中間產(chǎn)物,在臭氧氧化過程中發(fā)現(xiàn)10種不同質(zhì)荷比的中間產(chǎn)物。證明了在臭氧氧化中引進(jìn)電化學(xué)作用增強(qiáng)了AMO的降解。結(jié)合量子化學(xué)計算結(jié)果提出了AMO的不同降解途徑,包括苯甲酸環(huán)和氨基的降解,四元β內(nèi)酰胺環(huán)的開環(huán),硫的氧化及其它鍵裂解反應(yīng)。
[Abstract]:Antibiotics are widely used to treat human and animal diseases and to promote animal growth as feed additives. However, due to their potentially adverse effects on aquatic ecology and human health, Antibiotics in the natural environment, such as water bodies, are of particular concern. Because antibiotics are antibacterial and biotoxic, traditional biological water treatment methods can not effectively remove antibiotics from the environment. It is necessary to develop efficient treatment technology to remove antibiotics in water and reduce the impact of antibiotics on the environment. In this paper, amoxicillin AMO-wastewater was studied and electrochemical oxidation was used. Ozone oxidation and electrochemical combined ozone oxidation are used to treat them, and the effect and mechanism of ozone oxidation and electrochemical combined ozone oxidation are analyzed. Electrochemical combined ozonation is the most effective technique for AMO degradation. After 6 minutes of electrochemical action, only 37% of AMO can be removed, while in 5 minutes and 4 minutes, AMO can be completely treated by ozone and electrochemical combined ozone processes, respectively. In the salinity experiment, the total organic carbon salinity reached 67.8% after 60 minutes of electrochemical combined ozonation treatment. In comparison, only 47.3% and 3.1% of the total organic carbon mineralization were obtained by ozone oxidation and electrochemical treatment, respectively. The production of hydroxyl radical and the utilization rate of O3 have been improved in the process of electrochemical combined ozone oxidation. In order to control the amoxicillin process of electrochemical combined ozone treatment more economically and effectively. In this paper, the effects of some important operating parameters, such as ozone concentration and current pH, on the treatment efficiency of amoxicillin treated by electrochemical combined ozone are systematically studied. When the concentration of ozone in aeration increases during the electrochemical combined ozone oxidation process, the degradation of amoxicillin and the salinity of TOC are increased. When the current is increased from 100mA to 300mA, The degradation and TOC mineralization of amoxicillin increase with the increase of the applied current. However, when the current is further increased to 400mA, Amoxicillin degradation and TOC mineralization did not increase or even decrease to a certain extent. In this study, we found that H value plays an important role in AMO degradation and TOC mineralization, which not only affects the decomposition of ozone and the production of hydroxyl radical in aqueous solution. In addition, the mechanism of electrochemistry combined with ozone degradation of AMO was carried out. The results showed that the introduction of electrochemistry did promote the production of hydroxyl radicals. Therefore, the electrochemical combined ozonation process can degrade AMOO more economically and efficiently than ozonation. The degradation pathway of AMO was studied. The intermediates of electrochemical combined ozonation and ozonation alone were identified by UPLC-MS/MS technique. Fifteen intermediates with different charge ratios were found in electrochemical combined ozonation. In the process of ozone oxidation, 10 intermediates of different mass charge ratios were found. It was proved that the introduction of electrochemical action in ozone oxidation enhanced the degradation of AMO. Different degradation pathways of AMO were proposed in combination with quantum chemical calculations. These include the degradation of benzoic acid ring and amino group, the ring opening of quaternary 尾 -lactam ring, the oxidation of sulfur and other bond cleavage reactions.
【學(xué)位授予單位】：哈爾濱工業(yè)大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2015
【分類號】：X703

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本文編號：1673097