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研究生:劉益均
研究生(外文):Yi-Chun Liu
論文名稱:添加滑石粉及活性碳對Photo-Fenton降解乙醯胺基酚(ACE)之影響
論文名稱(外文):Degradation of acetaminophen with talc and activated carbon in wastewater by Photo-Fenton
指導教授:廖文彬廖文彬引用關係
指導教授(外文):Wing-Ping Liao
口試委員:謝永旭陳建隆
口試委員(外文):Yung-Hsu HsiehJiann-Long Chen
口試日期:2015-05-29
學位類別:碩士
校院名稱:國立中興大學
系所名稱:環境工程學系所
學門:工程學門
學類:環境工程學類
論文種類:學術論文
論文出版年:2015
畢業學年度:103
語文別:中文
論文頁數:124
中文關鍵詞:Photo-Fenton退熱止痛藥遮蔽滑石粉活性碳
外文關鍵詞:Photo-Fenton oxidation processAntipyretic and analgesic drugsShieldingTalcactivated carbon
相關次數:
  • 被引用被引用:3
  • 點閱點閱:85
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  • 下載下載:16
  • 收藏至我的研究室書目清單書目收藏:0
高級氧化程序(AOPs)為一種能夠產生強氧化力且非選擇性氫氧自由基(‧OH)的氧化處理程序,其被廣泛的運用於降解水中各種有機物汙染物。
本研究以乙醯胺基酚(acetaminophen, ACE)退熱止痛藥作為目標污染物,初始濃度為10mg/L,控制不同參數(H2O2濃度、Fe2+濃度、光強度等),利用五種氧化程序紫外光/過氧化氫(UV/H2O2)、亞鐵離子/過氧化氫(Fenton)、紫外光/亞鐵離子/過氧化氫(Photo-Fenton)、紫外光/亞鐵離子/過氧化氫/活石粉(Photo-Fenton/Talc)、紫外光/亞鐵離子/過氧化氫/活性碳(Photo-Fenton /AC),對廢水中ACE以及化學需氧量(COD)去除,並探討各程序間之影響與差異。
研究結果顯示,Fenton 程序之最適操作條件為pH = 3、[H2O2]/[Fe2+] = 0.99/0.066 mM時,ACE去除率為68.7%。在Photo-Fenton 程序之最適操作條件光強度 = 90 W、pH = 3、[H2O2]/[Fe2+] = 0.99/0.066 mM下,其ACE去除率為78.1%。UV/H2O2程序中,ACE去除率則為14.4%。在三種程序中
,不論是ACE或COD的去除率,皆以Photo-Fenton 程序為最佳。
此外,不論滑石粉或活性碳的添加皆會因為遮蔽或吸附效應之影響而使Photo-Fenton程序的去除成效下降,但若將活性碳(0.1 g/L)於反應60分鐘後再添加至系統中,可有效提升ACE之去除率,Photo-Fenton/Talc及Photo-Fenton/AC程序中ACE去除率各別為66.3%、85.8%。
在所有程序中,以Photo-Fenton/AC(60 min)程序具有最佳的ACE及COD去除效率,其中所增加之去除率為活性碳吸附作用所導致。


Advanced oxidation processes (AOPs) is a kind of oxidation processes which can produce strong oxidation ability, with non-specific hydroxyl radical
(.OH), and it is widely used to degrade a variety of organic pollutants in the wastewater. In the study, the pollutant initial concentration is 10 mg/L. The intention of research is in order to investigate the removal and chemical oxygen demand (COD) of Acetaminophen(ACE) antipyretic and analgesic drugs by UV/H2O2, Fenton, Photo-Fenton and Photo-Fenton/AC systems with controlling different parameter (H2O2 concentration, Fe2+ concentration, light intensity). Trying to discuss about the differences and effects between each process.
The results showed that, the optimal conditions for the removal rate of ACE (68.7%) were [H2O2]/[Fe2+] = 0.99/0.066 mM at pH 3 in the Fenton process. Photo-Fenton process with optimal parameters of UV light= 90 W, [H2O2]/[Fe2+]= 0.99/0.066 mM at pH 3, the ACE removal rate is 78.1%. As to the UV/H2O2 system, the ACE removal rate is 14.4%. In the three process, Photo-Fenton process has the best effect of the removal rate of either ACE or COD.
Additionally, either talc or activated carbon addition, the removal effect of Photo-Fenton process both reduced according to the influence of shielding or adsorption effect. However, the removal rate of ACE can be effectively enhanced by adding activated carbon in 60 minute after reaction. The removal rate of ACE in Photo-Fenton/Talc and Photo-Fenton/AC process were 66.3% and 85.8%, respectively.
Among all the processes, Photo-Fenton/AC(60 min) process has the best ACE and COD removal efficiency and the increase of removal rate results from adsorption effect by activated carbon.


目錄
摘要 I
Abstract II
目錄 III
表目錄 V
圖目錄 VI
第一章 前言 1
1-1 研究緣起 1
1-2 研究目的 2
1-3 研究內容 2
第二章 文獻回顧 4
2-1 新興污染物 4
2-2 個人保健醫藥用品 7
2-3 乙醯胺基酚之簡介 10
2-3-1 乙醯胺基酚之毒理機制與代謝 13
2-3-2 乙醯胺基酚之分解 15
2-3-3 乙醯胺基酚之相關文獻 17
2-4 UV/H2O2氧化處理程序 19
2-4-1 UV/H2O2程序簡介 20
2-4-2 UV/H2O2程序影響因子 21
2-5 Photo-Fenton氧化處理程序 24
2-5-1 Photo-Fenton降解有機物之機制 25
2-5-2 Photo-Fenton氧化處理之優缺點 26
2-5-3 Fenton氧化處理程序簡介 27
2-5-4 Fenton氧化處理之優缺點 30
2-5-5 Fenton及Photo-Fenton、Photo-Fenton/Talc、
Photo-Fenton/AC氧化處理程序影響因子 32
第三章 材料與方法 37
3-1 實驗設計 37
3-2 實驗操作 37
3-2-1 實驗操作方法 40
3-2-2 系統控制參數 43
3-3 實驗系統裝置 51
3-4 實驗藥品及配置 53
3-4-1 實驗藥品 53
3-4-2 實驗藥品配置 54
3-5 實驗設備 55
3-6 實驗分析方法 56
3-6-1 ACE濃度分析方法 56
3-6-2 過氧化氫分析方法 57
3-6-3 亞鐵離子濃度分析 58
3-6-4 COD分析方法 58
第四章 結果與討論 60
4-1 檢量線建立 60
4-2 ACE全波長分析 61
4-3 背景實驗 64
4-3-1 紫外光直接光解 64
4-3-2 過氧化氫直接氧化 66
4-3-3 亞鐵離子單獨添加 68
4-3-4 滑石粉單獨添加 70
4-3-5 活性碳單獨添加 72
4-4 UV/H2O2實驗 74
4-4-1 初始溶液pH效應 74
4-4-2 光照強度影響 77
4-5 Fenton實驗 78
4-6 Photo-Fenton實驗 83
4-7 Photo-Fenton/Talc實驗 88
4-8 Photo-Fenton/AC實驗 92
4-8-1 活性碳添加量效應 92
4-8-2 活性碳(低劑量)添加時間效應 98
4-8-3 活性碳(高劑量)添加時間效應 101
4-9 六系統比較 105
4-9-1 六系統降解及礦化之差異 105
4-9-2 六系統k值之比較 109
第五章 結論與建議 112
5-1 結論 112
5-2 建議 114
第六章 參考文獻 115
6-1 中文文獻 115
6-2 英文文獻 117
附錄 122

表目錄
表2- 1 常見的新興環境污染之PPCPs整理 8
表2- 2 2005/1~2006/12 國貿局 PPCPs 物質之進口量 9
表2- 3 Acetaminophen物理化學資料 10
表2- 4 2005年健保藥物使用統計量前二十大使用藥物 12
表2- 5 常見氧化劑之標準氧化還原電位 28
表2- 6 Fenton反應中可能的反應式和速率常數 29
表2- 7 系統pH值對Fenton反應之影響 32
表2- 8 各文獻之最佳 Fenton 試劑比值 33
表3- 1 背景實驗之操作參數 44
表3- 2 UV/H2O2實驗之操作參數 46
表3- 3 Fenton實驗之操作參數 47
表3- 4 Photo-Fenton實驗之操作參數 48
表3- 5 Photo-Fenton/Talc實驗之操作參數 49
表3- 6 Photo-Fenton/AC實驗之操作參數 50
表3- 7 實驗分析項目及方法 56
表4- 1 各分析項目檢量線 60
表4- 2 UV/H2O2、Fenton、Photo-Fenton、Photo-Fenton/Talc
Photo-Fenton/AC(0min)、Photo-Fenton/AC(60 min),六系統
之反應常數k值 110

圖目錄
圖2- 1 新興污染物簡易分類 5
圖2- 2 新興污染物進入環境的路徑 6
圖2- 3 新興污染物於自然界中之質量流示意圖 6
圖2- 4 實驗室乙醯胺基酚的合成 11
圖2- 5 乙醯胺酚於體內的代謝路徑圖 15
圖2- 6 乙醯氨基酚主要分解途徑 16
圖2- 7 隨溶液 pH 值不同過氧化氫之解離情形 19
圖3- 1 研究架構圖 38
圖3- 2 研究流程圖 39
圖3- 3 光反應器 52
圖4- 1 ACE於不同pH值下之UV光譜圖 61
圖4- 2 ACE (a)pH=3, (b)pH=5, (c)pH=7, (d) pH=9, (e)pH=11.7 63
圖4- 3 直接光解之(a)ACE濃度, (b)pH, (c)ORP 之變化圖 65
圖4- 4 過氧化氫氧化之(a)ACE濃度, (b)pH, (c)ORP 之變化圖 67
圖4- 5 亞鐵離子單獨添加之(a)ACE濃度, (b)pH, (c)ORP 之變化圖 69
圖4- 6 滑石粉單獨添加之(a)ACE濃度, (b)pH, (c)ORP 之變化圖 71
圖4- 7 活性碳單獨添加之(a)ACE濃度, (b)pH, (c)ORP 之變化圖 73
圖4- 8 UV/H2O2不同初始pH值之ACE去除率 75
圖4- 9 UV/H2O2不同初始pH值之(a)過氧化氫濃度, (b)pH值, (c)ORP值
之變化圖([ACE]=10 mg/L;[H2O2]=3.30 mM;光源=90 W;
pHi=3、5、6.86、9) 76
圖4- 10 UV/H2O2在不同光強度下反應,去除率隨時間之變化圖
([ACE]=10mg/L;[H2O2]=3.30 mM;光源=0、45、90 W;
pHi=3) 77
圖4- 11 Fenton反應於不同Fenton試劑添加劑量及比例下之ACE
去除率 80
圖4- 12 Fenton反應於不同Fenton試劑添加劑量及比例下之(a)過氧化氫
濃度, (b)亞鐵離子濃度, (c)pH值, (d)ORP值隨時間的變化趨勢圖
([ACE]=10 mg/L;pHi=3;反應時間=120 min) 82
圖4- 13 Photo-Fenton反應於不同Fenton試劑比例下之ACE去除率 84
圖4- 14 Photo-Fenton反應於不同Fenton試劑比例下之(a)過氧化氫濃
度, (b)亞鐵離子濃度, (c)pH值, (d)ORP值隨時間的變化趨勢圖
([ACE]=10 mg/L;[H2O2]=0.99 mg/L;pHi=3;反應時間=120
min;光源=90W) 86
圖4- 15 Photo-Fenton/ Talc實驗於不同滑石粉量添加下之ACE去除率 89
圖4- 16 滑石粉添加劑量與遮蔽效應之關係圖 90
圖4- 17 Photo-Fenton/ Talc實驗於不同滑石粉量添加下之(a)過氧化氫濃
度,(b)亞鐵離子濃度, (c)pH值, (d)ORP值隨時間的變化趨勢圖
([ACE]=10 mg/L;[H2O2]0 = 0.99 mM;[Fe2+]0 =0.066
mM;pHi=3;反應時間=120 min;UV lamp = 6支(90 W) ) 91
圖4- 18 Photo-Fenton/ AC實驗於不同活性碳量添加下之ACE去除率 93
圖4- 19 活性碳添加劑量與遮蔽及吸附效應之關係圖 94
圖4- 20 滑石粉及活性碳添加劑量與遮蔽及吸附效應之比較關係圖 95
圖4- 21 滑石粉及活性碳添加劑量與濁度之比較關係圖 95
圖4- 22 Photo-Fenton/ AC實驗於不同活性碳量添加下之(a)過氧化氫濃
度,(b)亞鐵離子濃度, (c)pH值, (d)ORP值隨時間的變化趨勢
([ACE]=10 mg/L;[H2O2]0 = 0.99 mM;[Fe2+]0 =0.066
mM;pHi=3;反應時間=120 min;UV lamp = 6支(90 W) ) 97
圖4- 23 Photo-Fenton/ AC實驗於活性碳(低劑量)不同時間添加下之
ACE去除率 99
圖4- 24 Photo-Fenton/ AC實驗於活性碳(低劑量)不同時間添加下之
(a)過氧化氫濃度, (b)亞鐵離子濃度, (c)pH值, (d)ORP值隨時間
的變化趨勢圖([ACE]=10 mg/L;[H2O2]0 = 0.99 mM;
[Fe2+]0 =0.066 mM;[AC]0 =0.01 g/L;pHi=3;反應時間
=120 min;UV lamp = 6支(90 W) ) 100
圖4- 25 Photo-Fenton/ AC實驗於活性碳(高劑量)不同時間添加下之
ACE去除率 103
圖4- 26 Photo-Fenton/ AC實驗於活性碳(高劑量)不同時間添加下之
(a)過氧化氫濃度, (b)亞鐵離子濃度, (c)pH值, (d)ORP值隨時間
的變化趨勢圖([ACE]=10 mg/L;[H2O2]0 = 0.99 mM;
[Fe2+]0 =0.066 mM;[AC]0 =0.1 g/L;pHi=3;
反應時間120 min;UV lamp = 6支(90 W) ) 104
圖4- 27 UV/H2O2、Fenton、Photo-Fenton、Photo-Fenton/Talc、
Photo-Fenton/AC(0 min)、Photo-Fenton/AC(60 min),六系
統於最佳及最具代表條件下反應之(a)ACE去除率,(b)COD去除率隨時間
的變化趨勢圖 107


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