以高級氧化程序礦化水中對-硝基苯酚之研究

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陳伯全(CHEN POCHUAN) 查詢紙本館藏

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以高級氧化程序礦化水中對-硝基苯酚之研究
(Using Advanced Oxidation Process to Mineralize p-Nitrophenol in Aqueous Solution)

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摘要(中)

本研究主要將含有p-Nitrophenol之溶液，以O3結合UV及H2O2之高級氧化程序進行礦化處理，並以總有機碳(Total Organic Carbon; TOC)作為p-Nitrophenol之礦化效率指標。於不同高級氧化程序， p-Nitrophenol礦化效率排序為：UV/O3＞UV/O3/H2O2＞O3＞O3/H2O2＞UV/H2O2，最佳p-Nitrophenol礦化效率之高級氧化程序為UV/O3程序(78.1%)。
於UV/O3程序，實驗結果顯示隨著H2O2注入劑量之增加， p-Nitrophenol之礦化效率隨之減少。H2O2在UV/O3程序主要扮演掠奪者之角色。於O3程序，控制H2O2注入劑量為0~31.60 mg/min，實驗結果顯示H2O2注入劑量3.95 mg/min時對p-Nitrophenol礦化提升之效率最為顯著，於UV/O3程序，分別控制反應過程之pH值為3.0~10.0，實驗結果顯示控制pH值時皆優於未控制pH值，其中pH值為10.0礦化效率最佳。另以初始反應濃度10~100 mg/L，實驗結果顯示隨著初始反應濃度增加，p-Nitrophenol礦化效率及轉化率隨之降低。
由實驗結果可觀察到UV/O3程序礦化p-Nitrophenol之過程並非單純之一階反應(First-order reaction)，而是擬一階反應(Pseudo first-order reaction)；擬一階反應常數(kobs)介於0.0032~0.0175 min-1之間，隨著H2O2注入劑量增加，擬一階反應常數(kobs)隨之降低；不同pH值之擬一階反應常數(kobs)介於0.0158~0.0291 min-1之間，控制pH值為10.0時具有最佳之反應速率；不同p-Nitrophenol初始反應濃度之擬一階反應常數(kobs)介於0.0134~0.0806 min-1之間。

摘要(英)

This present study aims to evaluate the performance of advanced oxidation processes that combines UV, O3 and H2O2 to mineralize p-Nitrophenol in aqueous solution. The concentration of total organic carbon (TOC) was selected as an efficiency index of p-Nitrophenol mineralization. For different advanced oxidation processes, the efficiency of p-Nitrophenol mineralization followed the sequence UV/O3＞UV/O3/H2O2＞O3＞O3/H2O2＞UV/H2O2. The UV/O3 process got the best 78.1% efficiency of p-Nitrophenol mineralization.
For the UV/O3 process, the results indicated that as the concentration of H2O2 increased, the rate of p-Nitrophenol mineralization declined. In other words, H2O2 acted as a scavenger of hydroxide radical ( ). While for the O3 process, it indicated that the efficiency of p-Nitrophenol mineralization is optimal when H2O2 dosage is 3.95 mg/min among .0 to 31.60 mg/min. Also for the UV/O3 process, the mineralization efficiency is optimal when pH was fixed to be 10.0 than pH was fixed below 10.0 or when pH was not fixed in oxidation process. When initial p-Nitrophenol concentration was controlled as 10~100 mg/L and pH was controlled as 10.0, it indicated that the efficiency of p-Nitrophenol mineralization declined as the initial p-Nitrophenol concentration increased. Hence, the mineralization rate of highly concentrated p-Nitrophenol was lower.
It is observed that process of p-Nitrophenol mineralized by UV/O3 is not just a simple first-order reaction but pseudo first-order reaction. The pseudo first-order rate constant (kobs) of different H2O2 dosage was calculated between 0.0032~0.0175 min-1. As the H2O2 increases, the reaction rate constant declined. The pseudo first-order rate constant (kobs) for pH among 3.0 to 10.0 was calculated to be between 0.0158~0.0291 min-1. Still, when pH was fixed to be10.0 the oxidation process got the best reaction rate constant. The pseudo first-order rate constant (kobs) for different initial p-Nitrophenol concentration was calculated between 0.0134~0.0806 min-1.

關鍵字(中)

★ 高級氧化
★ 臭氧
★ UV
★ p-Nitrophenol
★ 礦化效率

關鍵字(英)

★ Advanced oxidation
★ Ozone
★ UV
★ p-Nitrophenol
★ Mineralization efficiency

論文目次

目錄
摘　要 i
Abstract iii
誌　謝 v
目錄 vi
表目錄 x
圖目錄 xiii
第一章前　言 1
1.1 研究緣起 1
1.2 研究目的與內容 2
第二章文獻回顧 4
2.1 對-硝基苯酚之特性 4
2.1.1 對-硝基苯酚基本性質 4
2.1.2 對-硝基苯酚化學合成方式 5
2.1.3 對-硝基苯酚之用途 6
2.1.4 對-硝基苯酚對人體之危害 7
2.2 高級氧化程序介紹 8
2.2.1 臭氧基本性質 11
2.2.2 UV光基本性質 19
2.2.3 氫氧自由基基本性質 22
2.2.4 O3/UV高級氧化程序 23
2.2.5 O3/UV/H2O2高級氧化程序 24
2.3 高級氧化程序礦化苯酚類污染物之文獻 27
第三章實驗設備與方法 37
3.1 實驗設計 37
3.1.1 不同反應程序之礦化效率探討 37
3.1.2 不同反應條件之礦化效率探討 39
3.2 實驗系統架構與測試 41
3.2.1 實驗系統架構 41
3.2.2 實驗系統測試 41
3.3 實驗器材與藥品 44
3.3.1 實驗器材 44
3.3.2 實驗藥品 46
3.4 分析方法 47
3.4.1 氣相臭氧濃度分析方法 47
3.4.2 水中臭氧濃度分析方法 48
3.4.3 UV照射強度分析方法 49
3.4.4 總有機碳分析方法 50
第四章結果與討論 52
4.1 不同氧化程序對p-Nitrophenol之礦化效率探討 52
4.1.1 UV礦化p-Nitrophenol之效率 52
4.1.2 H2O2礦化p-Nitrophenol之效率 54
4.1.3 O3礦化p-Nitrophenol之效率 56
4.1.4 UV/H2O2礦化p-Nitrophenol之效率 58
4.1.5 O3/ H2O2礦化p-Nitrophenol之效率 60
4.1.6 UV/O3礦化p-Nitrophenol之效率 62
4.1.7 UV/O3/H2O2礦化p-Nitrophenol之效率 64
4.1.8 不同氧化程序礦化p-Nitrophenol彙整說明 66
4.2 不同反應條件礦化p-Nitrophenol效率之探討 69
4.2.1 H2O2注入劑量對p-Nitrophenol礦化效率之影響 69
4.2.2 pH值對UV/O3程序礦化p-Nitrophenol效率之影響 79
4.2.3 p-Nitrophenol初始反應濃度對UV/O3程序礦化效率之影響 83
4.2.4 不同氧化程序礦化p-Nitrophenol彙整說明 87
4.3 程序礦化p-Nitrophenol之反應動力關係探討 89
4.3.1 不同H2O2注入劑量對UV/O3程序礦化p-Nitrophenol之反應動力關係探討 89
4.3.2 UV/O3程序於不同pH值條件下礦化p-Nitrophenol之反應動力關係探討 91
4.3.3 UV/O3程序對不同p-Nitrophenol初始反應濃度之反應動力關係探討 93
4.3.4 程序礦化p-Nitrophenol之反應動力關係彙整說明 94
第五章結論與建議 96
5.1 結論 96
5.2 建議 100
參考文獻 101
附錄一 105
附錄二 107
表目錄
表2.1.1-1　對-硝基苯酚之基本物理化學性質 5
表2.2-1　各式氧化劑氧化能力比較表 9
表2.2-2　各種高級氧化法之自由基型態 11
表2.2.1-1　臭氧基本物理特性 13
表2.2.1-2　臭氧水解動力階數一覽表 19
表3.2.2-1　臭氧注入劑量測試結果 43
表3.2.2-2　水中臭氧濃度測試結果 43
表3.2.2-3　UV光強度量測結果 43
表3.3.1-1　實驗器材一覽表 44
表3.3.2-1　實驗藥品一覽表 46
表4.1.1-1　UV礦化p-Nitrophenol實驗結果 53
表4.1.2-1　 H2O2礦化p-Nitrophenol實驗結果 55
表4.1.3-1　O3礦化p-Nitrophenol實驗結果 57
表4.1.4-1　UV/H2O2程序礦化p-Nitrophenol實驗結果 59
表4.1.5-1　O3/H2O2程序礦化p-Nitrophenol實驗結果 61
表4.1.6-1　UV/O3程序礦化p-Nitrophenol實驗結果 63
表4.1.7-1　UV/O3/H2O2程序礦化p-Nitrophenol實驗結果 65
表4.2.1-1　UV/O3程序於不同H2O2劑量之實驗結果 70
表4.2.1-1　UV/O3程序於不同H2O2劑量之實驗結果(續) 71
表4.2.1-1　UV/O3程序於不同H2O2劑量之實驗結果(續) 72
表4.2.1-2　O3程序於不同H2O2劑量之實驗結果 75
表4.2.1-2　O3程序於不同H2O2劑量之實驗結果(續) 76
表4.2.1-2　O3程序於不同H2O2劑量之實驗結果(續) 77
表4.2.2-1　不同pH值對UV/O3程序礦化p-Nitrophenol之實驗結果 80
表4.2.2-1　不同pH值對UV/O3程序礦化p-Nitrophenol之實驗結果(續) 81
表4.2.3-1　UV/O3程序對不同p-Nitrophenol初始反應濃度之實驗結果 84
表4.2.3-1　UV/O3程序對不同p-Nitrophenol初始反應濃度之實驗結果(續) 85
表4.3.1-1　UV/O3程序於不同H2O2劑量礦化p-Nitrophenol之擬一階反應常數(kobs)與相關係數(R2) 91
表4.3.2-1　UV/O3程序於不同pH值礦化p-Nitrophenol之擬一階反應常數(kobs)與相關係數(R2) 92
表4.3.3-1　UV/O3程序於不同p-Nitrophenol初始反應濃度之擬一階反應常數(kobs)與相關係數(R2) 94

圖目錄

圖2.1.1-1　p-Nitrophenol之化學結構圖 4
圖2.1.4-1　對-硝基苯酚於人體內之代謝途徑 8
圖2.2.1-1　臭氧之化學結構圖 11
圖2.2.1-2　電暈放電製造臭氧之基本原理示意圖 15
圖2.2.1-3　水中臭氧氧化化合物之直接與間接反應路徑 15
圖2.2.1-4　電偶極加成反應(Criegee mechanism)示意圖 16
圖2.2.1-5　親電性反應(Electrophilic reaction)示意圖 17
圖2.2.1-6　臭氧與芳香烴有機物(Aromatic compounds)反應示意圖 17
圖2.2.1-7　臭氧分解路徑示意圖(Staehelin et al., 1984) 18
圖2.2.1-8　臭氧自由基連鎖反應誘使者、提升者及抑制者之定義 18
圖2.2.3-1　UV光電磁頻譜(Electromagnetic Spectrum)分類圖 20
圖2.2.3-2　UV光於水中傳送之相關影響機制示意圖 22
圖2.2.4-1　UV(254 nm)裂解臭氧之反應路徑 24
圖2.2.5-1　O3/UV/H2O2系統之反應途徑 25
圖2.3-1　臭氧氧化酚之反應機制及中間產物 27
圖2.3-2　臭氧氧化1,3-苯二酚及1,3,5-苯三酚之反應路徑及中間產物 28
圖2.3-3　臭氧氧化酚之反應機制及中間產物 29
圖2.3-4　臭氧氧化2-氯酚、3-氯酚之反應機制及中間產物 30
圖2.3-5　臭氧氧化對-羥基苯甲酸之反應機制及中間產物 31
圖2.3-6　2,4-DP之氧化反應機制及中間產物 34
圖3.2.1-1　本研究之實驗儀器裝置示意圖 42
圖3.4.1-1　氣相臭氧分析儀(GM-pro) 47
圖3.4.2-1　溶臭氧分析儀(Dissolved Ozone Monitor) 48
圖3.4.3-1　UV光強度偵測示意圖 49
圖3.4.4-1　TOC分析儀(Dohrmann Phoenix 8000)分析流程圖 50
圖4.1.1-1　UV礦化p-Nitrophenol之效率 53
圖4.1.2-1　H2O2礦化p-Nitrophenol之效率 55
圖4.1.3-1　O3礦化p-Nitrophenol之效率 57
圖4.1.4-1　UV/H2O2程序礦化p-Nitrophenol之效率 59
圖4.1.5-1　O3/H2O2程序礦化p-Nitrophenol之效率 61
圖4.1.6-1　UV/O3程序礦化p-Nitrophenol之效率 63
圖4.1.7-1　UV/O3/H2O2程序礦化p-Nitrophenol之效率 65
圖4.1.8-1　不同氧化程序p-Nitrophenol礦化效率比較 66
圖4.1.8-2　不同氧化程序之p-Nitrophenol轉化率比較 67
圖4.1.8-3　不同氧化程序反應過程之pH值變化情形 68
圖4.2.1-1　UV/O3程序於不同H2O2劑量之p-Nitrophenol礦化效率 73
圖4.2.1-2　UV/O3程序於不同H2O2劑量之p-Nitrophenol轉化率 73
圖4.2.1-3　O3程序於不同H2O2劑量之p-Nitrophenol礦化效率 78
圖4.2.1-4　O3程序於不同H2O2劑量之p-Nitrophenol轉化率 78
圖4.2.2-1　UV/O3程序於不同pH值之p-Nitrophenol礦化效率 82
圖4.2.2-2　UV/O3程序於不同pH值之p-Nitrophenol轉化率 82
圖4.2.3-1　UV/O3程序對不同p-Nitrophenol初始反應濃度之礦化效率 86
圖4.2.3-2　UV/O3程序對不同p-Nitrophenol初始反應濃度之轉化率 86
圖4.3.1-1　UV/O3程序於不同H2O2劑量之p-Nitrophenol礦化速率 90
圖4.3.2-1　UV/O3程序於不同pH值之p-Nitrophenol礦化速率 92
圖4.3.2-1　UV/O3程序於不同p-Nitrophenol初始反應濃度之礦化速率 93

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指導教授

莊銘棟

審核日期

2014-7-24

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