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研究生:謝一誠
研究生(外文):I-Chen Hsieh
論文名稱:鐵氧化物催化過氧化氫氧化2-硝基酚之研究
論文名稱(外文):DESTRUCTION OF 2-NITROPHENOL BY IRON OXIDES CATALYZED HYDROGEN PEROXIDE
指導教授:張祖恩張祖恩引用關係
指導教授(外文):Juu-En Chang
學位類別:碩士
校院名稱:國立成功大學
系所名稱:環境工程學系
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:1999
畢業學年度:87
語文別:中文
論文頁數:103
中文關鍵詞:鐵氧化物過氧化氫催化氧化2-硝基酚
外文關鍵詞:Iron oxideshydrogen peroxidecatalytic oxidation2-nitrophenol
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本研究利用鐵氧化物催化過氧化氫探討此法對2-硝基酚破壞去除之效果。實驗中改變鐵氧化物種類、劑量及過氧化氫濃度等因子以觀察其對2-硝基酚破壞效率之影響。實驗結果發現在pH為3的控制條件下以針鐵礦(α-FeOOH)、赤鐵礦(Fe2O3)以及磁鐵礦(Fe3O4)三種鐵氧化物催化過氧化氫氧化2-硝基酚時,α-FeOOH與Fe3O4皆有催化過氧化氫氧化2-硝基酚之成效,且2-硝基酚氧化破壞效率隨過氧化氫濃度與鐵氧化物劑量之增加而增加,其在本研究最佳的操作條件下皆可分別在1小時及3小時下完全去除2-硝基酚;至於Fe2O3則幾乎沒有催化過氧化氫氧化2-硝基酚之效果。在催化實驗過程中,本研究發現Fe2O3沒有亞鐵溶出的情況,其總鐵溶出亦較少且沒有持續溶出的現象,而α-FeOOH及Fe3O4皆有鐵離子依零階反應動力模式之持續溶出的情形,且亞鐵離子濃度佔大部份比例。此表示以α-FeOOH及Fe3O4催化過氧化氫之反應過程中,在液相裡可能有以亞鐵離子型態進行的Fenton反應發生,促使2-硝基酚的氧化破壞。為釐清在鐵氧化物催化過氧化氫破壞2-硝基酚過程中固液相催化氧化之反應比例,經以外加亞鐵離子方式模擬鐵氧化物之鐵溶出現象進行過氧化氫催化反應,結果發現Fe3O4表面極可能有異相催化H2O2氧化2-硝基酚之能力,但α-FeOOH則主要是由鐵溶出所產生之液相催化效應為主。

ABSTRACT
Catalysis of hydrogen peroxide had been conducted by iron oxides, includingα-FeOOH, Fe2O3, and Fe3O4, to investigate the efficiency for the destruction of 2-nitrophenol (2-NP). Several types of and dosage of iron oxide and concentration of hydrogen peroxide on the 2-NP destruction efficiency had also been discussed in this study. The results show thatα-FeOOH and Fe3O4 could effectively catalyze hydrogen peroxide to destroy 2-NP, and the 2-NP destruction efficiency was improved by increasing the iron oxide dosage and concentration of hydrogen peroxide, but not Fe2O3. During the destruction of 2-NP by the catalytic reactions of hydrogen peroxide, dissolution of ferrous ion from the iron oxides could be found. Consequently, the catalysis of hydrogen peroxide for the destruction of 2-NP by iron oxide can be characterized by two mechanisms. A heterogeneous catalysis mechanism is that hydrogen peroxide is catalyzed by solid phase on the iron oxide surface, and the homogeneous catalysis system means that hydrogen peroxide is catalyzed by the ferrous ion dissolved from iron oxide. In this study, it was found that heterogeneous system was predominant for the catalysis of hydrogen peroxide by Fe3O4, while homogeneous catalysis was significant as α-FeOOH had been used. Nevertheless, the destruction of 2-NP by homogeneous catalysis of hydrogen peroxide was faster than by heterogeneous catalysis system.

授權書…………………………………………I
簽署人須知…………………………………………II
考試合格證書…………………………………………III
中文摘要…………………………………………IV
英文摘要…………………………………………V
誌謝…………………………………………VI
目錄…………………………………………VII
表目錄…………………………………………XI
圖目錄…………………………………………XIII
第一章 前言…………………………………………1
1-1 研究動機…………………………………………1
1-2 研究目的與方法…………………………………………3
第二章 文獻回顧…………………………………………4
2-1 硝酚類化合物及其處理方法………………………………………4
2-1-1 硝酚類化合物之來源與特性………………………………4
2-1-2 硝酚類化合物之處理方法…………………………………5
2-1-2-1 生物處理法…………………………………………6
2-1-2-2 物理處理程序…………………………………………9
2-1-2-3 高級氧化法…………………………………………9
2-2 鐵氧化物之基本特性及其應用………………………………17
2-2-1 鐵氧化物之種類…………………………………………17
2-2-2 鐵氧化物的應用…………………………………………18
2-3 H2O2催化氧化系統之原理與應用…………………………………………24
2-3-1 UV/H2O2系統之原理與應用………………………………25
2-3-2 Fenton Reagent法…………………………………………26
2-3-3 H2O2/鐵氧化物之異相催化………………………………28
第三章 實驗設備、材料與方法…………………………………………30
3-1 實驗設備…………………………………………30
3-1-1 催化氧化實驗設備…………………………………………30
3-1-2 水質分析設備…………………………………………30
3-1-3 鐵氧化物製備及其特性分析設備…………………………33
3-2 實驗材料…………………………………………33
3-2-1 鐵氧化物前處理…………………………………………33
3-2-2 人工配製廢水…………………………………………33
3-3 實驗方法…………………………………………34
3-3-1 針鐵礦之合成方法…………………………………………34
3-3-2 BET比表面積之測定……………………………………34
3-3-3 採樣分析項目及方法………………………………………34
3-4 實驗步驟…………………………………………35
3-4-1 背景實驗…………………………………………35
3-4-2 催化氧化實驗…………………………………………36
第四章 結果與討論…………………………………………39
4-1 Fenton法氧化2-硝基酚…………………………………………39
4-1-1 過氧化氫氧化2-硝基酚之效果……………………………39
4-1-2 Fenton法氧化2-硝基酚之效果………………………………40
4-2 鐵氧化物催化過氧化氫氧化2-硝基酚…………………………………43
4-2-1 α-FeOOH催化過氧化氫氧化2-硝基酚之行為………………………43
4-2-1-1 α-FeOOH 對2-硝基酚之吸附行為………………………………43
4-2-1-2 α-FeOOH 劑量之影響…………………………………………46
4-2-1-3 過氧化氫濃度之影響……………………………………48
4-2-2 Fe3O4催化氧化2-硝基酚之行為……………………………………51
4-2-2-1 Fe3O4對2-硝基酚之吸附行為……………………………………51
4-2-2-2 Fe3O4劑量之影響…………………………………………53
4-2-2-3 過氧化氫濃度之影響………………………………………55
4-2-3 Fe2O3催化過氧化氫氧化2-硝基酚之行為…………………………57
4-2-3-1 Fe2O3對2-硝基酚之吸附行為……………………………………57
4-2-3-2 Fe2O3劑量之影響……………………………………60
4-2-3-3 過氧化氫濃度之影響…………………………………………61
4-2-4 三種鐵氧化物催化氧化2-硝基酚之綜合討論………63
4-3 鐵溶出對鐵氧化物催化過氧化氫氧化反應之影響……………………66
4-3-1 異相催化反應之鐵溶出行為……………………………66
4-3-2 溶鐵速率對於異相催化反應之影響…………………………………77
4-4 鐵氧化物催化過氧化氫氧化2-硝基酚之反應情形探討………………80
第五章 結論與建議…………………………………………89
5-1 結論…………………………………………89
5-2 建議………………………………………………………………90
參考文獻……………………………………………………………92
附錄………………………………………………………………100
自述………………………………………………………………103

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