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研究生: 邱翌竹
Chiou, Yi-Chu
論文名稱: 動物用抗生素於畜牧廢水厭氧及好氧處理程序中生物降解潛勢與中間產物之評估
Biodegradation of Veterinary Antibiotics and Intermediate Products during Aerobic and Anaerobic Processes for Livestock Wastewater Treatment
指導教授: 黃良銘
Whang, Liang-Ming
陳婉如
Chen, Wan-Ru
學位類別: 碩士
Master
系所名稱: 工學院 - 環境工程學系
Department of Environmental Engineering
論文出版年: 2016
畢業學年度: 104
語文別: 英文
論文頁數: 143
中文關鍵詞: 巨環內酯類抗生素林克醯胺類抗生素四環素類抗生素磺胺類抗生素吸附
外文關鍵詞: Macrolides, Lincosamides, Tetracyclines, Sulfonamides, Adsorption
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  • 水資源匱乏逐年加劇,造成嚴重問題,而畜牧廢水量佔全台灣廢水比例超過25 %,又其富含氮磷營養源,是極具有發展潛勢的農業再利用水來源。然而,其中殘留之抗生素並不能被傳統廢水處理程序移除,隨廢水被排放入環境中的抗生素將造成生態破壞甚至促使抗藥性基因的產生及擴散,對人類的健康產生極大威脅。本研究針對兩座畜牧廢水處理廠進行調查,定期檢測四環素類、磺胺類、林可醯胺類以及巨環黴素類共十種抗生素在各處理單元之出現頻率以及去除情形做探討;架設實驗室規模之連續批分次反應槽模擬實場,定期添加抗生素馴養污泥,另外厭氧及好氧反應槽皆設置未添加抗生素作為實驗對照組;此外以批次試驗釐清各物質對抗生素的個別影響。Lincomycin (LCM)、Tylosin (TYL)以及Erythromycin (ERY) 被選定釐清傳統生物處理程序中,其吸附、吸收效應與生物降解能力,同時與四種常用的磺胺類抗生素Sulfadiazine (SDZ)、Sulfathiazole (STZ)、Sulfamerazine (SMR)與Sulfamethoxazole (SMX)及三種四環素類抗生素Tetracycline (TC)、Oxytetracycline (OTC)、Chlortetracycline (CTC)之結果比較。在批次試驗中的結果顯示,畜牧廢水並不會對於ERY及四種磺胺類造成吸附或是分析上的影響,而四環素類抗生素則會被吸附於畜牧廢水,LCM與TYL所受到影響則相對四環素輕微。而在污泥與抗生素吸附的測試當中,發現LCM、TYL、ERY與STZ的與濃度會輕微下降,四環素類抗生素會大量且快速的被污泥吸附,SDZ、SMR和SMX皆未發現與污泥之間有吸附行為。在生物降解的測試結果顯示,長期暴露於抗生素之污泥具有較強的生物降解抗生素的潛力, TYL與ERY與具有好氧及厭氧生物降解能力,LCM僅具有好氧生物降解能力,四種磺胺類也皆可於好氧處理程序中降解,SMX也被發現具有厭氧生物降解能力。而四環素類抗生素並未顯示具有好氧生物降解潛勢。除此之外,在厭氧處理程序中,ERY被發現了兩個中間產物(m/z皆為734),SMX也被發現了兩個中間產物(m/z為212及254)。

    Water scarcity causes serious problems. Therefore, developing more water sources such as reclaimed waters are urgent. Livestock wastewater accounting for 26 % of overall wastewater in Taiwan and containing high concentration of nutrient is a potential source of reclaimed water for agriculture. However, traditional wastewater treatments could not totally remove antibiotics contented in livestock wastewater. Antibiotics discharged into environment will cause ecological damages and increase antibiotic resistances in microorganisms. Two livestock wastewater treatment plants were investigated the occurrences and the removal efficiencies of antibiotics regularly. Lab-scale sequencing batch reactors were built to simulate the treatment processes, part of them were added with antibiotics and others were used as control group without additional antibiotics. Then, batch tests were conducted to assess the effects and removal mechanism of antibiotics in biological treatment process. Moreover, possible metabolites during biological process would be confirmed by LC-MS/MS. In this study, the adsorption behavior and biodegradation of lincomycin (LCM), tylosin (TYL) and erythromycin (ERY) were investigated. The biotic and abiotic behaviors of tetracycline (TC), oxytetracycline (OTC), chlortetracycline (CTC) sulfadiazine (SDZ), sulfathiazole (STZ), sulfamerazine (SMR) and sulfamethoxazole (SMX) were summarized and discussed. The results of batch tests showed that tetracyclines were largely affected by wastewater and sludge while LCM, TYL, ERY and STZ were slightly affected and the interaction of SDZ, SMR and SMX with wastewater matrix could be neglected. Moreover, TYL, ERY and SMX had anaerobic biodegradation potential. There were no aerobic biodegradation potential for tetracycline antibiotics and no anaerobic biodegradation potential for LCM. Furthermore, there were two intermediate products at m/z 734 for ERY and two intermediate products at m/z 212 and 254 for SMX found in anaerobic condition. Overall, this study could help to clarify the fate and behavior of ten antibiotics in the aerobic and anaerobic process.

    摘要 I Abstract III Acknowledgements V Table of Content IX List of Tables XV List of Figures XIX Chapter 1 Introduction 1 Chapter 2 Literature Review 3 2-1 Water Resources 3 2-2 Livestock wastewater 3 2-2-1 The characteristics of livestock wastewater 4 2-2-2 Recycling of nutrients from livestock wastewater 4 2-2-3 Livestock wastewater treatment process 5 2-3 Emerging contaminants 5 2-4 Antibiotics 6 2-4-1 Usage of antibiotics 6 2-4-2 The fates of antibiotics in environment 11 2-4-3 Resistance and toxicity of antibiotics 14 2-4-4 The veterinary antibiotics commonly used 17 2-5 Removal of antibiotics in biological treatment system 19 2-5-1 Biodegradation 19 2-5-2 Biosorption 21 2-6 Metabolites and degradation products of antibiotics 23 Chapter 3 Materials and Methods 25 3-1 Research framework 25 3-2 Livestock wastewater treatments 26 3-3 Antibiotics 28 3-4 Water quality analysis 33 3-5 Gas production analysis 34 3-6 Antibiotics analysis 34 3-6-1 High performance liquid chromatography with UV/Vis detector (HPLC-UV) 34 3-6-2 Liquid chromatography-tandem mass spectrometry (LC-MS/MS) 35 3-7 Excitation/Emission Matrix Spectrofluorometer (EEMs) 37 3-8 Laboratory-scale sequencing batch reactors 38 3-8-1 Aerobic Sequencing Batch Reactor (SBR) 38 3-8-2 Anaerobic Sequencing Batch Reactor (ASBR) 40 3-9 Batch experiment 42 3-9-1 The abiotic removal test of antibiotics 44 3-9-2 The biodegradation test of antibiotics 46 Chapter 4 Results and Discussion 51 4-1 Livestock wastewater analysis 51 4-1-1 Monitoring results of treatment plant A 51 4-1-2 Monitoring results of treatment plant B 55 4-2 Lab-scale aerobic sequencing batch reactors (SBRs) 59 4-2-1 The performance of SBR with LCM, TYL and ERY (SBR-LET) 59 4-2-2 Bioactivity of aerobic reactor with/without antibiotics 62 4-3 Lab-scale anaerobic sequencing batch reactors (ASBRs) 65 4-3-1 The performance of ASBR with LCM, TYL and ERY (ASBR-LET) 65 4-3-2 ASBR bioreactor adding tylosin, erythromycin and sulfamethoxazole (ASBR-ETS) 67 4-3-3 Bioactivity of anaerobic reactor with/without antibiotics 70 4-4 The abiotic removal of antibiotics 75 4-4-1 Abiotic batch tests with anaerobic livestock wastewater 75 4-4-2 Abiotic batch tests with aerobic reactor supernatant 80 4-4-3 Abiotic batch tests with sludge 85 4-4-4 Summary 89 4-5 Biodegradation of antibiotics 94 4-5-1 Biodegradation batch of antibiotics under aerobic condition 94 4-5-2 Biodegradation batch of antibiotics under anaerobic condition 105 4-5-3 Summary 111 4-6 Intermediate products of antibiotics 115 4-7 Discussion 123 Chapter 5 Conclusions and Suggestions 131 5-1 Conclusions 131 5-1-1 Full-scale livestock wastewater treatment plants 131 5-1-2 Lab-scale SBR and ASBR bioreactors 131 5-1-3 The non-biological distribution of antibiotics 132 5-1-4 The biological distribution of antibiotics 132 5-1-5 Intermediate products of antibiotics 132 5-2 Suggestions 133 References 135

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