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研究生:鄭慈儀
研究生(外文):Tzu-Yi Cheng
論文名稱:利用不同氧化程序以礦化四甲基氫氧化銨之研究
論文名稱(外文):Mineralization of Tetramethylammonium Hydroxide in Aqueous Solution by Different Oxidation Processes
指導教授:邱求三
指導教授(外文):Chyow-San Chiou
口試委員:邱求三陳華偉洪桂彬
口試委員(外文):Chyow-San ChiouHua-Wei Chen,Kuei-Pin Hung
口試日期:2013-06-01
學位類別:碩士
校院名稱:國立宜蘭大學
系所名稱:環境工程學系碩士班
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:2013
畢業學年度:101
語文別:中文
論文頁數:109
中文關鍵詞:礦化作用紫外光/臭氧四甲基氫氧化銨高級氧化程序
外文關鍵詞:mineralizationUV/O3Tetramethylammonium hydroxideadvanced oxidation process.
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四甲基氫氧化銨Tetramethylammonium Hydroxide (TMAH) 廣泛使用於薄膜晶體管液晶顯示器TFT-LCD(Thin Film Transistor Liquid Crystal Display)及半導體產業製程中。因TMAH具毒性且不易被生物降解,故其排放前須經特殊廢水處理程序。本文旨在O3、O3/UV、O3/H2O2/UV與不同催化劑(均相及非均相)程序,用於礦化TMAH並評估其礦化效率及最佳條件。
  其中臭氧程序處理液相有機污染物在應用方面,受限於臭氧在水中溶解度及其處理效果。因此,本研究嘗試使用均相催化(FeSO4/O3),以及非均相催化(MnO2/O3)並嘗試使用UV光以及過氧化氫程序礦化TMAH。
  從實驗結果可知礦化效果依順序為:UV/O3>H2O2/UV/O3>MnO2/O3>FeSO4/O3>O3,UV/O3系統礦化TMAH的降解效果最好,且在pH10有最佳的礦化效果達87.1%。

Tetramethylammonium hydroxide (TMAH) is widely used in thin-film transistor liquid crystal display (TFT-LCD) and semiconductor processing industries. Because of its toxicity, wastewater containing TMAH has to be undergone a proper treatment before discharge. The objective of this study was using advanced oxidation processes (O3, O3/UV, and O3/H2O2/UV) with homogeneous and heterogeneous catalyst to mineralize TMAH and evaluate the optimum reaction conditions and its mineralization efficiency.
The mineralization efficiency of TMAH under various processes followed the sequence: UV/O3>H2O2/UV/O3>MnO2/O3>FeSO4/O3>O3. The mineralization efficiency was up to 87.1% of UV/O3 with the reaction solution pH at 10.

目錄
摘要 I
Abstract II
第一章 緒論 1
1.1 研究緣起 1
1.2研究目的與內容 3
第二章 文獻回顧 4
2.1 TFT-LCD廢水的基本性質 4
2.1.1液晶顯示器製程廢水與處理技術 4
2.3二氧化錳簡介 11
2.3.1二氧化錳來源及性質 11
2.3.2二氧化錳用途 13
2.3.3 錳氧化物相關之文獻整理 13
2.4臭氧氧化程序 18
2.4.1簡述各種氧化程序 18
2.4.2臭氧(O3)的基本性質 18
2.4.3臭氧在水溶液中的質傳理論 21
2.4.4在水溶液中臭氧的自解機制及動力行為 25
2.4.5影響廢污水臭氧氧化之因子 28
2.4.6溶液pH值對臭氧反應的影響 29
2.5過氧化氫(H2O2)基本性質 30
2.5.1過氧化氫/臭氧氧化反應 31
2.6紫外光催化反應 34
2.6.1光化學反應 34
2.6.2光化學反應類型 36
2.6.3紫外光/臭氧氧化程序 37
2.6.4紫外光/過氧化氫氧化程序 41
2.6.5紫外光/觸媒氧化程序 41
2.7觸媒催化程序 42
2.7.1均相催化 42
2.7.2非均相催化 45
2.7.3非均相改質型 51
第三章 材料與方法 54
3.1 實驗藥品與儀器 54
3.1.1實驗藥品 54
3.1.2儀器 55
3.2特性分析 57
3.2.1 XRD分析 57
3.2.2 Flame-AAS分析 57
3.3 實驗裝置 58
3.4 實驗步驟 60
3.5實驗架構 62
3.6分析測定方法 63
3.6.1氣相臭氧濃度分析 63
3.6.2總有機碳(TOC)濃度分析 65
3.6.3錳離子濃度分析 66
3.6.4鐵離子濃度分析 67
3.6.5過氧化氫濃度分析 68
第四章 結果與討論 69
4.1不同pH值條件下O3程序對TMAH之礦化影響 69
4.2均相觸媒催化 71
4.2.1 FeSO4在不同pH條件下對TMAH礦化速率的影響 71
4.2.2 FeSO4/O3不同添加量對TMAH礦化速率的影響 73
4.3 非均相觸媒催化 75
4.3.1 MnO2/O3在不同pH條件下對TMAH礦化速率的影響 75
4.3.2 MnO2的添加量對反應程序之探討 77
4.3.3 MnO2性質之討論 80
4.3.3.1 XRD分析 80
4.4探討UV/O3程序在不同pH值對礦化TMAH之影響 81
4.4.1 pH與TOC/TOC0對時間之關係 81
4.4.2 UV/O3程序反應環境pH值對TMAH礦化效率的影響 81
4.5探討UV /O 3/ H2O2程序中礦化TMAH礦化速率的影響 84
4.5.1 H2O2添加量對礦化TMAH的影響 84
4.7 UV/O3 程序下TMAH濃度對反應程序之探討 89
4.7.1 TMAH濃度對礦化速率之影響 89
4.7.2動力模式探討 89
4.8.1 UV/O3程序中氯鹽與硫酸鹽對礦化TMAH之干擾 92
第五章 結論 94
5.1 結論 94
參考文獻 96


圖目錄
圖1-1 Tetramethylammonium Hydroxide化學結構圖 2
圖2-1光電產業廢水分類 4
圖2-2 TFT製程與廢水來源流程圖 9
圖2-3 LCD製程與廢水來源流程圖 10
圖2-4臭氧的共振結構(Cotton et al., 1966) 18
圖2-5臭氧在不同共振態的分子軌域 19
圖2-6雙膜理論示意圖 21
圖2-7臭氧質傳與化學反應速率關係(Charpentier,1981) 24
圖2-8臭氧自解示意圖(Staehelin et al., 1984) 27
圖2-9臭氧自解過程中的光解反應機制﹙Peyton and Glaze,1988﹚ 40
圖2-10觸媒吸附有機物後再藉由臭氧或氫氧基氧化反應機制圖(Legube et al., 1999) 47
圖2-11臭氧與金屬觸媒反應後進行氧化作用之反應機制圖(Legube et al., 1999) 48
圖3-1高級氧化系統設備裝置圖 59
圖3-2實驗架構圖 62
圖3-3以UV分析O3濃度之檢量線 64
圖3-4以TOC分析總有機碳濃度之檢量線 65
圖3-5以原子吸收光譜儀(AA)分析錳離子濃度之檢量線 66
圖3-6以原子吸收光譜儀(AA)分析鐵離子濃度之檢量線 67
圖3-7以分光光度計分析過氧化氫濃度之檢量線 68
圖4-1為不同pH條件下O3程序對TMAH的礦化效率圖 70
圖4-2 FeSO4/O3不同反應環境pH值對於TMAH的降解速率圖 72
圖4-3 FeSO4不同添加量對於TMAH的降解速率圖 74
圖4-4 MnO2/O3不同反應環境pH值對於TMAH的礦化速率圖 76
圖4-5不同MnO2添加量對TMAH礦化速率 79
圖4-6為不同型態的MnO2的XRD圖譜 80
圖4-7 pH與TOC/TOC0與時間之關係圖 82
圖4-8 UV/O3不同反應環境pH值對於TMAH的礦化效率圖 83
圖4-9為不同劑量H2O2條件下結合UV/O3程序對TMAH的礦化效率圖 85
圖4-10 O3、O3/UV、O3/H2O2/UV與不同催化劑(均相及非均相)在臭氧程序中礦化TMAH之關係圖 88
圖4-11 不同起始濃度之TMAH降解速率圖 90
圖4-12 不同起始濃度之TMAH礦化動力模式圖 91


表目錄
表1-1 Tetramethylammonium Hydroxide 化學特性表 2
表2-1 TFT-LCD產業主要廢棄物清理現況彙整 (鄭志和,2005) 6
表2-2為錳氧化物在不同溫度之型態 12
表2-3為MnO2與不同程序之整理表 17
表2-4臭氧的基本性質(Cotton , 1966) 20
表2-5各種氧化劑之還原電位(Prengle and Mauk , 1978) 20
表2-6臭氧自解動力式的文獻整理,(張介林,1995) 26
表2-7影響臭氧氧化之無機離子 28
表2-8 過氧化氫之物化性質 (顧洋,1993) 30
表2-9溶液pH值對過氧化氫/臭氧反應程序影響之文獻 33
表2-10化學鍵的斷裂能量,(Legan , 1982) 35
表2-11均向催化程序文獻整理 44
表2-12非均相催化劑的分類*表示為較不重要之功能)  (胡興中,1991) 46
表2-13非均相催化程序之文獻 50
表2-14非均相改質催化程序之文獻 53
表3-1控制因子實驗項目略表 60
表3-2反應動力實驗各實驗項目 61
表3-4原子吸收光譜儀錳離子分析設定 66
表3-5鐵離子分析設定 67
表3-6過氧化氫分析設定 68
表4-1不同pH之條件下反應60分鐘之鐵離子濃度 72
表4-2不同FeSO4添加量反應60分鐘之鐵離子濃度 74
表4-3不同pH之條件下反應60分鐘之錳離子濃度 76
表4-4不同MnO2添加量反應60分鐘之錳離子濃度 79
表4-5 不同起始濃度對TMAH的降解速率常數之影響 91
表4-6 影響臭氧氧化之無機離子 93
表4-7 UV/O3程序中添加無機離子反應60分鐘之礦化表 93


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