紫外光/過氧化氫程序降解辛基苯酚聚氧乙烯醇水溶液之研究

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蔡維馨(Wei-Sin Tsai) 查詢紙本館藏

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論文名稱

紫外光/過氧化氫程序降解辛基苯酚聚氧乙烯醇水溶液之研究
(Degradation of OPEOn in Aqueous Solution by UV/H2O2 Process)

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摘要(中)

本研究以紫外光/過氧化氫程序處理辛基苯酚聚氧乙烯醇(Octylphenol polyethoxylates, OPEOn)水溶液，並探討溶液pH、反應物初始濃度、光輻射強度及過氧化氫添加量等操作因子對處理效果之影響，以及，探討OPEOn於紫外光/過氧化氫程序可能之降解途徑，最後，評估環境中常見之無機陰離子對降解程序之影響。
實驗結果顯示，3小時反應時間內，直接光解和H2O2直接氧化均無法有效去除溶液中OPEOn，而UV/H2O2程序可在反應90分鐘後，達到90%以上之去除率，但無法有效去除水中總有機碳含量，原因是UV/H2O2程序僅能破壞OPEOn原本的結構，而無法進一步將其礦化成二氧化碳和水。
溶液中碳酸鹽和硝酸鹽的存在，均會顯著降低OPEOn的降解速率，這是因為兩者均可捕捉系統內的氫氧自由基所致。此外，碳酸鹽對程序之影響和其濃度無關，而硝酸鹽對程序之影響則和其存在的濃度有關聯。
由LC/MS分析中間產物之結果顯示，OPEOn降解由聚乙氧基鏈開始，而後氫氧自由基可能會添加至芳香環上，或是取代烷基上的氫，以及削減烷基鏈。降解過程中所生成之中間產物，包括：短鏈烷基苯酚聚氧乙烯醇、醛類化合物以及有機酸等。
本研究初步認為，以UV/H2O2程序降解OPEOn，其最適操作條件為：光強度=0.89 W/L，pH=7，H2O2/OPEOn=10。此操作條件下，反應90分鐘後，OPEOn可達95%去除率及15%之礦化效果。

摘要(英)

This study evaluates the treatment of octylphenol polyethoxylates (OPEOn) solution using UV/H2O2 process. The influences of pH, initial substrate concentration, H2O2 dosage and photon fluence rate in OPEOn degradation were studied. Also, possible degradation mechanism of OPEOn in UV/H2O2 process was proposed. Finally, assess the effect of inorganic salts, such as NaNO3 and Na2CO3, on OPEOn degradation.
Relatively slow OPEOn degradation was observed during UV radiation, while OPEOn was not oxidized by H2O2 along. Combined UV/H2O2 could effectively degraded OPEOn, and resulted in more than 90% removal of OPEOn in 90 min period. However, removal of total organic carbon in solution was ineffective. The results indicated that OPEOn was destroyed and formation numerous of intermediate products, but can’t converted to CO2 and H2O by mineralization.
The presence of NaNO3 and Na2CO3 in solution led to decreased the degradation rate of OPEOn. This may be attributed to the scavenging of hydroxyl radical by these two inorganic anions. Besides, the effect of NaNO3 was depend on the concentration of anion.
The degradation products were analyzed by LC/MS, and revealed that OPEOn degradation begin from shortening the ethoxy chain. And the following may be cleavage of the alkyl chain, or substitution of the hydrogen on alkyl chain with hydroxyl radical, as well as addition hydroxyl radical to the aromatic ring. The degradation intermediates are short chain ethoxylated phenol, aldehydic compounds and organic acid.
In summary, the optimum operating conditions for UV/H2O2 process to destroy OPEOn found in this study was as follows：UV light intensity = 0.89 W/L, pH=7, H2O2/OPEOn molar ratio = 10. In which, a treatment effectiveness of 95% was achieved after 90 minutes of reaction time, and 15% mineralization was obtained .

關鍵字(中)

★ 內分泌干擾物
★ 高級氧化程序
★ 紫外光/過氧化氫
★ 辛基苯酚聚氧乙烯醇

關鍵字(英)

★ Endocrine disrupting compound
★ Advanced oxidation process
★ Octylphenol polyethoxylates
★ Ultraviolet irradiation/hydrogen peroxide

論文目次

摘要 I
Abstract II
誌謝 IV
目錄 III
圖目錄 VII
表目錄 X
第一章前言 1
1.1 研究緣起 1
1.2 研究目的 2
第二章文獻回顧 4
2.1 新興污染物-內分泌干擾物 4
2.2 烷基苯酚聚氧乙烯醇類界面活性劑之性質、流佈與影響 7
2.3 烷基苯酚聚氧乙烯醇及其代謝物常見之處理方式 13
2.4 過氧化氫/紫外光程序 16
2.4.1 紫外光氧化程序 17
2.4.2 過氧化氫特性 17
2.4.3 氫氧自由基氧化 18
2.5 過氧化氫/紫外光程序之影響因子 20
2.5.1 酸鹼值 20
2.5.2 輻射光強度 21
2.5.3 過氧化氫起始濃度 22
2.5.4 目標污染物起始濃度 23
2.5.5 自由基捕捉劑 (Scanvenger) 24
2.6 烷基苯酚聚氧乙烯醇類界面活性劑之降解途徑 25
2.6.1 生物降解 26
2.6.2 直接光解 28
2.6.3 高級氧化 29
第三章實驗設備、材料及方法 33
3.1 實驗儀器 33
3.2 實驗藥品 34
3.3 實驗設備裝置 35
3.4 實驗方法 37
3.5 分析方法 40
第四章結果與討論 46
4.1 背景試驗 46
4.1.1 光強度試驗 46
4.1.2 過氧化氫氧化試驗 47
4.1.3 直接光解實驗 49
4.1.4 綜合討論 54
4.2 紫外光/過氧化氫程序分解辛基苯酚聚氧乙烯醇界面活性劑 56
4.2.1 起始溶液pH效應 56
4.2.2 過氧化氫添加量效應 62
4.2.3 輻射光強度效應 67
4.2.4 反應物初始濃度效應 70
4.2.5 綜合討論 76
4.3 反應動力之探討 78
4.3.1 二階反應速率常數之推算 78
4.3.2 雙指數動力模式之探討 85
4.4 無機離子抑制效應評估 87
4.4.1 碳酸鹽濃度影響 87
4.4.2 硝酸鹽濃度影響 90
4.4.3 綜合討論 94
4.5 辛基苯酚聚氧乙烯醇降解途徑之探討 96
第五章結論與建議 107
5.1 結論 107
5.2 建議 109
References 110

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指導教授

曾迪華(Dyi-Hwa Tseng)

審核日期

2011-7-22

推文