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系統識別號 U0026-2208201715085500
論文名稱(中文) 雌激素與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之評估
論文名稱(英文) Biodegradation of Estrogens and Veterinary Antibiotics during Aerobic and Anaerobic Processes for Livestock Wastewater Treatment
校院名稱 成功大學
系所名稱(中) 環境工程學系
系所名稱(英) Department of Environmental Engineering
學年度 105
學期 2
出版年 106
研究生(中文) 蘇哲立
研究生(英文) Je-Li Su
學號 P56044071
學位類別 碩士
語文別 英文
論文頁數 184頁
口試委員 指導教授-黃良銘
指導教授-陳婉如
口試委員-林財富
口試委員-周佩欣
中文關鍵字 雌激素  磺胺類抗生素  四環素類抗生素  林克醯胺類抗生素  巨環內酯類抗生素  生物降解 
英文關鍵字 Estrogens  Sulfonamides  Tetracyclines  Lincosamides  Macrolides  Biodegradation 
學科別分類
中文摘要 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27 %,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,其中殘留之雌激素與動物用抗生素並不能被傳統廢水處理程序有效移除,隨廢水被排放入環境中的雌激素形成內分泌干擾物,影響動物體內內分泌系統的正常運作;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,定期檢測三種雌激素以及四環素類、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,定期添加雌激素或抗生素馴養污泥,另外厭氧及好氧反應槽皆設置未添加任何雌激素與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。Estrone (E1)、17β-estradiol (E2)以及Estriol (E3) 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)、Sulfamethoxazole (SMX)以及三種四環素類抗生素Tetracycline (TC)、Oxytetracycline (OTC)、Chlortetracycline (CTC)以及兩種巨環內酯類抗生素Tylosin (TYL)、Erythromycin (ERY)以及林可醯胺類抗生素Lincomycin (LCM)之結果比較。此外,在之前研究中Sulfadiazine (SDZ)、Sulfathiazole (STZ)、Sulfamerazine (SMR)、Tetracycline (TC)、Oxytetracycline (OTC)以及Chlortetracycline (CTC)未完成厭氧生物降解潛勢之評估,也會在本研究中進行充分的實驗與釐清。在批次試驗中的結果顯示,畜牧廢水與汙泥會顯著吸附吸收四環素類抗生素,而汙泥則是會顯著吸附吸收E1與E2。畜牧廢水並不會對於三種雌激素、ERY與四種磺胺類造成吸附或是分析上的影響,LCM與TYL所受到影響則相對四環素輕微。LCM、TYL、ERY與STZ受到汙泥的吸附吸收濃度會輕微下降,E3、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,雌激素、磺胺類抗生素、LCM、TYL以及ERY有好氧生物降解的潛勢,而E2、TYL、ERY與SMX則是有厭氧生物降解的潛勢。四環素類抗生素沒有生物降解潛勢,而E1、E3、LCM、SDZ、STZ與SMR則是沒有厭氧生物降解潛勢。
英文摘要 Water scarcity causes serious problems. Thus, developing more water resources for reuse becomes an important issue. Livestock wastewater accounting for 27% of overall wastewater in Taiwan and containing high concentration of nitrogen and phosphate nutrients is a potential source of fertilizer for agriculture. Nevertheless, conventional wastewater treatment plants could not remove estrogens and antibiotics contented in livestock wastewater efficiently. Estrogens discharged into environment will disrupt normal endocrine system function of animals, while antibiotics discharged into environment will increase antibiotics resistances in microorganisms. Two livestock wastewater treatment plants (LWTPs) were investigated the occurrence of estrogens and antibiotics regularly. Lab-scale sequencing batch reactors were built to simulate the treatment processes, part of them were spiked with estrogens or antibiotics and others were used as control group without additional estrogens and antibiotics. Then, batch tests were conducted to clarify removal mechanisms of estrogens and antibiotics in biological treatment process. In the study, the sorption behavior and biodegradation of estrone (E1), 17β-estradiol (E2), and estriol (E3) were investigated. The biotic and abiotic behaviors of tetracycline (TC), oxytetracycline (OTC), chlortetracycline (CTC), sulfadiazine (SDZ), sulfathiazole (STZ), sulfamerazine (SMR), sulfamethoxazole (SMX), lincomycin (LCM), tylosin (TYL) and erythromycin (ERY) were summarized and discussed. Besides, the unfished part of anaerobic biodegradability of tetracycline (TC), oxytetracycline (OTC), chlortetracycline (CTC) sulfadiazine (SDZ), sulfathiazole (STZ) and sulfamerazine (SMR) in previous studies were also clarified. The results of batch tests showed that tetracyclines were largely affected by wastewater and sludge while E1 and E2 were significantly affected by sludge. LCM, TYL, ERY and STZ were slightly affected and the interaction of E3, SDZ, SMR and SMX with wastewater matrix could be neglected. Moreover, estrogens, sulfonamides, LCM, TYL and ERY had aerobic biodegradation potential while E2, TYL, ERY and SMX had anaerobic biodegradation potential. There were no biodegradation potential for tetracyclines and no anaerobic biodegradation potential for E1, E3, LCM, SDZ, STZ and SMR. Overall, this study could help to clarify the fate and behavior of three estrogens and ten antibiotics in the aerobic and anaerobic biological treatment process.
論文目次 Table of Content
摘要 I
Abstract III
誌謝 V
Acknowledgements IX
Table of Content XI
List of Tables XVII
List of Figures XXI
Chapter 1 Introduction 1
Chapter 2 Literature Review 3
2-1 Livestock wastewater 3
2-1-1 The characteristics of livestock wastewater 3
2-1-2 Recycling of nutrients from livestock wastewater 4
2-1-3 Livestock wastewater treatment process 4
2-2 Emerging contaminants 5
2-3 Estrogens 5
2-3-1 The function of estrogens 6
2-3-2 The excretion of estrogens 6
2-3-3 The occurrences of estrogens in environment 8
2-3-4 Endocrine disrupting chemicals 11
2-4 Antibiotics 13
2-4-1 The usage of antibiotics 13
2-4-2 The occurrences of antibiotics in environment 18
2-4-3 Resistance and toxicity of antibiotics 20
2-4-4 The veterinary antibiotics commonly used 22
2-5 Removal of estrogens in biological treatment system 25
2-5-1 Biosorption 25
2-5-2 Biodegradation 26
2-6 Removal of antibiotics in biological treatment system 27
2-6-1 Biosorption 28
2-6-2 Biodegradation 29
2-7 Target emerging contaminants in this study 30
2-7-1 Estrogens 30
2-7-2 Antibiotics 32
Chapter 3 Materials and Methods 39
3-1 Research framework 39
3-2 Livestock wastewater treatments 40
3-3 Water quality analysis 42
3-4 Gas production analysis 43
3-5 Estrogens and antibiotics analysis 43
3-5-1 High performance liquid chromatography with UV/Vis detector (HPLC-UV) 43
3-5-2 Liquid chromatography-tandem mass spectrometry (LC-MS/MS) 44
3-6 Excitation/Emission Matrix Spectrofluorometer (EEMs) 47
3-7 Laboratory-scale sequencing batch reactors 48
3-7-1 Aerobic Sequencing Batch Reactor (SBR) 49
3-7-2 Anaerobic Sequencing Batch Reactor (ASBR) 50
3-8 Batch experiment 52
3-8-1 The abiotic removal test of estrogens and antibiotics 54
3-8-2 The biodegradation test of estrogens and antibiotics 57
Chapter 4 Results and Discussion 64
4-1 Livestock wastewater analysis 64
4-1-1 Monitoring results of treatment plant A 64
4-1-2 Monitoring results of treatment plant B 70
4-2 Lab-scale aerobic sequencing batch reactors (SBRs) 77
4-2-1 The performance of SBR with E1, E2 and E3 (SBR-Est) 77
4-2-2 Bioactivity of aerobic reactor with/without estrogens 82
4-3 Lab-scale anaerobic sequencing batch reactors (ASBRs) 87
4-3-1 The performance of ASBR with E1, E2 and E3 (ASBR-Est) 87
4-3-2 The performance of ASBR with SDZ, STZ and SMR (ASBR-SAs) 90
4-3-3 The performance of ASBR with TC, OTC and CTC (ASBR-TCs) 92
4-3-4 Bioactivity of anaerobic reactor with/without estrogens and antibiotics 94
4-4 The abiotic removal of estrogens and antibiotics 96
4-4-1 Abiotic batch tests with anaerobic livestock wastewater 96
4-4-2 Abiotic batch tests with aerobic reactor supernatant 103
4-4-3 Abiotic batch tests with sludge 110
4-4-4 Summary 117
4-5 Biodegradation of estrogens and antibiotics 123
4-5-1 Biodegradation batch of estrogens and antibiotics under aerobic condition 123
4-5-2 Biodegradation batch of estrogens under anoxic condition 134
4-5-3 Biodegradation batch of estrogens and antibiotics under anaerobic condition 136
4-5-4 Summary 144
4-6 Discussion 150
Chapter 5 Conclusions and Suggestions 164
5-1 Conclusions 164
5-1-1 Full-scale livestock wastewater treatment plants 164
5-1-2 Lab-scale SBR and ASBR bioreactors 164
5-1-3 The non-biological distribution of estrogens and antibiotics 165
5-1-4 The biological distribution of estrogens and antibiotics 165
5-2 Suggestions 166
References 168



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