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博碩士論文 etd-0703118-162127 詳細資訊
Title page for etd-0703118-162127
論文名稱
Title
添加氧化石墨烯複合材料於厭氧氨氧化系統對藥品去除與亞硝胺生成潛勢之影響
Impact of graphene oxide composites on the removal of pharmaceuticals and formation-potentials of nitrosamines during anaerobic ammonium oxidation
系所名稱
Department
畢業學年期
Year, semester
語文別
Language
學位類別
Degree
頁數
Number of pages
128
研究生
Author
指導教授
Advisor
召集委員
Convenor
口試委員
Advisory Committee
口試日期
Date of Exam
2018-07-19
繳交日期
Date of Submission
2018-08-03
關鍵字
Keywords
活性碳、厭氧氨氧化、氧化石墨烯、藥品、氨氮、亞硝酸氮、亞硝胺
Pharmaceutical, Nitrite, Anaerobic ammonium oxidation, Nitrosamine, Graphene oxide, Ammonia
統計
Statistics
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中文摘要
隨著工商業快速發展,人為活動所產生之廢污水組成趨於複雜,含氮磷之污染物與微量藥品與個人保健用品(Pharmaceuticals and personal care products,PPCPs)排放至環境水體中增加水中氮磷污染,導致水體發生優養化現象(Eutrophication)危害水中生態,且微量藥品存在於環境水體中若被汲取作為飲用水之原水,於消毒單元可能與消毒劑反應生成消毒副產物(Disinfection byproducts,DBPs),進一步提高對人體健康之危害。厭氧氨氧化技術(Anaerobic ammonium oxidation,Anammox)為一套快速發展之新穎廢污水處理技術,有別於傳統生物脫氮,為以無機碳作為碳源之化學自營性細菌,利用亞硝酸氮與氨氮做為電子接受與供給者,於厭氧條件下將兩者同時轉換為氮氣,具有污泥產生量低、少量有機碳供給、以及無需耗能曝氣等優點。本研究採用序批式間歇反應器(Sequencing batch reactor,SBR)建置厭氧氨氧化反應槽,由於Anammox代謝生長緩慢,故藉由SBR特性提高容積負荷(Volumetric loading)並減緩衝擊負荷(Shock loading),並嘗試於本系統添加石墨烯材料(Graphene oxide)刺激其生長,此外也測試以本系統降解國內使用量高之糖尿病藥物二甲雙胍(Metformin)及難生物降解之抗癲癇藥物卡馬西平(Carbamazepine),以其濃度變化與亞硝胺生成潛勢評估去除效率。本研究結果顯示,在無機氮去除部分,若氨氮與亞硝酸氮濃度提高時(200 mg/L),將使去除率下降至32%及54%,說明提高無機氮濃度可能抑制Anammox之生物活性;在藥品去除部分,因GO表面有大量含氧官能基團加快電子傳遞特性,使添加氧化石墨烯-四氧化三鐵(GO/Fe3O4)的系統,更能提高去除無機氮及Metformin,而Carbamazepine含芳香族環狀結構且屬於接受電子官能基團(Electron acceptor groups,EWGs)特性,導致生物較難降解,並由實驗結果推測其去除機制中吸附效果大於生物降解;亞硝胺生成潛勢之實驗中,添加活性碳或氧化石墨烯-四氧化三鐵都使亞硝胺類化合物濃度上升,Metformin中以NPyr、NMOR、NDBA為主要生成物種,則Carbamazepine是以NPyr、NPip、NMOR、NDBA為主要物種。
Abstract
With the technical and medical progresses in the last decades, pollutions of nitrogen and pharmaceuticals and personal care products (PPCPs) have been increasingly observed in water environments. Besides the adverse effects such as eutrophication caused by the occurrence of these contaminants, PPCPs are likely form carcinogenic disinfection byproducts (DBPs) such as nitrosamines during disinfection, causing harm to human health risks. Anaerobic ammonium oxidation (Anammox) is a novel biotechnology with the benefit of chemoautotrophic bacteria. In the process, organics is converted into carbon dioxide with ammonium and nitrite being the electron acceptors and being converted into inert N2 in an anaerobic environment. The major advantages of anammox include low sludge production, small amount of organic carbon supply, and limited aeration, et al. Sequencing batch reactor (SBR) was used in this study to establish the anammox reactor, due to the slow growth in metabolism of anammox bacteria. The SBR can effectively increase the volume loading and decrease the shocking loading. In addition, graphene-containing materials were added in the reactors to stimulate the growth of anammox bacteria. The feasibility to degrade the domestically used diabetes drug, Metformin, and the biodegradable antiepileptic drug, Carbamazepine, was another concern of this study, as the removal efficiencies of two pharmaceuticals and their nitrosamine formation potentials. The results show that when concentration of ammonia and nitrite were increased to 200 mg/L, the removal rate decreased to 32% and 54%, respectively, indicating that increasing the nitrogen input concentration may inhibit the biological activity. The anammox process is capable to treat metformin in waters, as the addition of graphene oxide composite (GO/Fe3O4) in the reactor improved the removals of both inorganic nitrogen and metformin. Carbamazepine, with its aromatic structure and electron withdraw groups (EWGs), was more difficultly degradable. Interestingly, adsorption and desorption, rather than biodegradation, may determine the fate of carbamazepine during anammox process. As to the variation of nitrosamine formation potentials, the addition of activated carbon or GO/Fe3O4 composite increases the concentrations of nitrosamine formation potentials. The main nitrosamine species formed by metformin contained N-Nitrosopyrrolidine(NPyr), N-Nitrosomorpholine(NMOR)andN-Nitrosodi-n-butylamine(NDBA), while carbamazepine mainly produced NPyr, N-Nitrosopiperidine(NPip), NMOR and NDBA.
目次 Table of Contents
論文審定書..................................................................................................................... i
摘要.............................................................................................................................. ii
Abstract .......................................................................................................................... iv
目錄.............................................................................................................................. vi
圖目錄........................................................................................................................... x
表目錄......................................................................................................................... xiii
第一章 前言.................................................................................................................. 1
1.1. 研究緣起................................................................................................................ 1
1.2. 研究目的................................................................................................................ 3
第二章 文獻回顧.......................................................................................................... 5
2.1. 氮循環及影響........................................................................................................ 5
2.2. 生物處理................................................................................................................ 7
2.3. 厭氧氨氧化............................................................................................................ 9
2.3.1. 厭氧氨氧化影響因素 ...................................................................................... 10
2.3.2. 生物去除含氮污染物之方法 .......................................................................... 12
2.3.3. 厭氧氨氧化反應槽與廢污水處理之應用 ...................................................... 15
2.4. 藥品...................................................................................................................... 16
2.4.1. 環境宿命與流佈 .............................................................................................. 17
2.4.2. 藥品環境與健康危害 ...................................................................................... 18
2.4.3. 處理程序與技術 .............................................................................................. 18
2.5. 亞硝胺類化合物.................................................................................................. 20
2.5.1. 環境流佈 .......................................................................................................... 22
2.5.2. 管制規範 .......................................................................................................... 22
2.5.3. 生成途徑與反應機制 ...................................................................................... 24
2.6. 活性碳.................................................................................................................. 28
2.7. 氧化石墨烯.......................................................................................................... 28
第三章 實驗材料與方法............................................................................................ 30
3.1. 研究架構.............................................................................................................. 30
3.2. 實驗材料與設備.................................................................................................. 32
3.2.1. 氧化石墨烯水溶液製備 .................................................................................. 32
3.2.2. 氧化石墨烯-四氧化三鐵複合材料製備 ........................................................ 32
3.2.3. 實驗試劑 .......................................................................................................... 33
3.2.4. 實驗設備 .......................................................................................................... 38
3.3. 儀器分析方法...................................................................................................... 39
3.3.1. 水質分析 .......................................................................................................... 39
3.3.2. 藥品前處理分析 .............................................................................................. 40
3.3.3. 亞硝胺類化合物前處理分析 .......................................................................... 42
3.4. 儀器介紹.............................................................................................................. 43
3.5. 微生物體16S 定序分析(16S Amplicon Sequencing) ................................... 44
3.6. 實驗流程.............................................................................................................. 45
3.6.1. Anammox 進行 SBR 馴養試驗 ..................................................................... 45
3.6.2. Anammox 添加載體及氧化石墨烯試驗 ........................................................ 47
3.6.3. 馴養完成測試去除藥品試驗 .......................................................................... 47
3.6.4. 藥品脫附試驗 .................................................................................................. 47
3.6.5. 亞硝胺生成潛勢試驗 ...................................................................................... 47
第四章 結果與討論.................................................................................................... 49
4.1. 以SBR 進行Anammox 之馴養 ......................................................................... 50
4.1.1. 水質變化(pH、ORP、EC、DO) .............................................................. 50
4.1.2. 無機氮之去除及生成 ...................................................................................... 54
4.1.3. 氨氮消耗、亞硝酸鹽氮消耗、與硝酸鹽氮生成之化學計量 ...................... 55
4.1.4. 氮負荷變化 ...................................................................................................... 56
4.2. 添加GO 對馴養過程之影響 .............................................................................. 58
4.2.1. 水質變化(pH、ORP、EC、 DO) ............................................................ 58
4.2.2. 無機氮之去除及生成 ...................................................................................... 61
4.2.3. 氨氮消耗、亞硝酸鹽氮消耗、與硝酸鹽氮生成之化學計量 ...................... 62
4.2.4. 反應槽氮負荷變化 .......................................................................................... 63
4.3. 在馴養期間添加GAC 或GO 對Anammox 產氣速率之影響 ........................ 65
4.4. 微生物體 16S 定序分析 ................................................................................... 66
4.5. Anammox 降解Metformin 之成效探討 ............................................................ 68
4.5.1. 添加Metformin 之pH、ORP、EC 變化 ....................................................... 68
4.5.2. 添加Metformin 於不同反應槽之無機氮變化 .............................................. 70
4.5.3. 添加Metformin 於不同反應槽之凱氏氮與總氮變化 .................................. 74
4.5.4. 添加Metformin 於不同反應槽之溶解性有機碳變化 .................................. 76
4.6. Anammox 添加Carbamazepine 之成效探討 ..................................................... 78
4.6.1. 添加Carbamazepine 之pH、ORP、EC 變化 ............................................... 78
4.6.2. 添加Carbamazepine 之無機氮濃度變化 ....................................................... 80
4.6.3. 添加Carbamazepine 之凱氏氮與總氮變化 ................................................... 84
4.6.4. 添加Carbamazepine 之溶解性有機碳變化 ................................................... 86
4.7. 添加不同載體之Anammox 污泥對藥品之去除及脫附 ................................... 88
4.7.1. 添加不同載體之Anammox 之藥品去除 ....................................................... 88
4.7.2. 添加不同載體之Anammox 反應槽中之藥品脫附可能 ............................... 91
4.8. 不同類型反應槽對亞硝胺之生成潛勢變化...................................................... 94
第五章 結論與建議.................................................................................................... 99
5.1. 結論...................................................................................................................... 99
5.2. 建議.................................................................................................................... 101
參考文獻.................................................................................................................... 102
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