臺灣博碩士論文加值系統

現今大量的廢棄污泥成為一種嚴重的環境問題。廢棄污泥中含有高濃度之內分泌干擾物—4-壬基苯酚 (4-Nonylphenol, 4-NP)。本研究使用木質素生物炭 (Lignin Biochar, LGBC)及改質LGBC結合氧化劑—過氧化鈣 (Calcium Peroxide, CaO2; CP)進行污泥中4-NP的氧化降解之研究。主要內容包含 (1) 於CO2、N2氣氛及熱解溫度300–900 °C下製備LGBC，並以最佳熱解條件製備改質LGBC，並利用傅立葉轉換紅外線光譜儀、界達電位測試儀進行材料特性分析；(2) 藉由CP氧化降解污泥中4-NP；(3) 探討LGBC和改質LGBC催化CP降解污泥中4-NP之降解能力。由傅立葉轉換紅外線光譜儀分析結果顯示，LGBC及改質LGBC表面皆具有大量的官能基。界達電位分析結果顯示，其pHzpc (零電荷點)約為1.2–3.7，在高於pHzpc的pH值帶有負電荷且電位大，說明LGBC及改質LGBC於鹼性環境分散性佳。氧化降解實驗結果表示，在CP濃度3.1×10-4 M時對4-NP之去除率約20 %；在CP濃度3.1×10-4 M、pH0 =11.0、溫度25 °C、劑量3.0 g/L之實驗條件下，以N2、700 °C熱解之LGBC催化CP降解污泥中的4-NP之降解率約80 %；於相同實驗條件下，使用NS改質LGBC作為催化劑，催化CP降解污泥中4-NP之去除率可提升至約84 %，且主要作用之自由基包含氫氧自由基 (HO•)及非自由基—單態氧 (1O2)。因此，由研究結果得知，利用高級氧化法處理受4-NP富集的污泥為可行之方式，且研究證明透過非金屬改質LGBC可以有效提升LGBC之催化能力，以達到循環經濟之效果。

A large amount of waste sludge has become a serious environmental problem. Waste sludge contains high concentrations of 4-Nonylphenol (4-NP), an endocrine disruptor. This study used Lignin Biochar (LGBC) and doped Lignin Biochar combined with Calcium Peroxide (CaO2; CP) to study the oxidative degradation of 4-NP in sludge. The primary research includes (1) LGBC synthesized at pyrolysis temperature of 300–900 °C as a catalytic material under nitrogen or carbon dioxide atmosphere, and preparation of doped LGBC under optimum pyrolysis conditions, then the material properties were analyzed by Fourier-transform infrared spectroscopy and zeta potential analyzer; (2) using CP to degrade 4-NP in sludge; (3) LGBC and doped LGBC activated CP to degrade 4-NP in sludge. The FTIR results showed that the surface of LGBC has many functional groups. The results of zeta potential analysis showed that its pHpzc (point of zero charges) is about 1.2–3.7, resulting that LGBC and doped LGBC are negatively charged at pH values higher than pHpzc. The oxidation experiments showed that under the experimental conditions of CP concentration of 3.1×10-4 M, the degradation rate of 4-NP in sludge about 20%. If under the experimental conditions of CP concentration of 3.1×10-4 M, pH0 =11.0, a temperature of 25 °C, and LGBC700 dosage of 3.0 g/L, the degradation rate of 4-NP in sludge can reach 80%; and if under the experimental conditions of same, using NS-LGBC, the degradation rate of 4-NP in sludge can reach 84%. Therefore, this research showed that the use of an advanced oxidation procedure to treat 4-NP-rich sludge is a feasible method. Research is showed that improve the catalytic ability and recycling effect of LGBC through doped LGBC to achieve the impact of the economic cycle.

摘要 i
Abstract ii
誌謝 iv
目錄 vi
圖目錄 x
附錄 xii
第一章 前言 1
1.1研究緣起 1
1.2研究目的 3
第二章 文獻回顧 4
2.1 4-壬基苯酚介紹 4
2.1.1壬基苯酚來源及傳播途徑 4
2.1.2 4-壬基苯酚之基本性質 5
2.1.3 4-壬基苯酚之危害影響 6
2.2高級氧化程序 7
2.2.1氧化劑之種類 8
2.2.2過氧化鈣的化學反應機制與應用 10
2.3生物炭 12
2.3.1生物炭 12
2.3.2木質素生物炭 13
2.3.3改質木質素生物炭 14
第三章 材料與方法 16
3.1研究架構 16
3.2實驗藥品與設備 17
3.2.1實驗藥品 17
3.2.2實驗設備 19
3.3污泥樣品採集 20
3.4生物炭製備 21
3.4.1木質素原始樣品前處理 21
3.4.2木質素生物炭製備方法 21
3.4.3改質木質素生物炭製備方法 21
3.5污泥中4-NP氧化降解反應 22
3.6 4-壬基苯酚分析 23
3.6.1定性及定量 23
3.6.2檢量線—4-壬基苯酚 24
3.7基本分析 25
3.7.1傅立葉轉換紅外光譜儀 25
3.7.2界達電位測試儀 26
第四章 結果與討論 27
4.1生物炭之基本分析 27
4.1.1傅立葉轉換紅外光譜儀—生物炭官能基分析 27
4.1.2界達電位測試儀—生物炭電位分析 30
4.2 CP氧化降解污泥中4-NP 35
4.2.1 CP濃度效應 35
4.3木質素生物炭催化CP降解污泥中4-NP 37
4.3.1熱解溫度效應 37
4.3.2劑量效應 39
4.3.3初始pH值效應 41
4.3.4反應基質濃度效應 43
4.3.5自由基捕捉試驗 45
4.4非金屬改質木質素生物炭催化CP降解污泥中4-NP 47
4.4.1各種非金屬元素改質木質素生物炭 47
4.4.2劑量效應 49
4.4.3初始pH值效應 51
4.4.4反應基質濃度效應 53
4.4.5自由基捕捉試驗 55
4.5複合金屬催化CP降解污泥中4-NP 57
4.5.1不同比例複合金屬 57
4.5.2劑量效應 59
4.5.3初始pH值效應 61
4.5.4反應基質濃度效應 63
4.5.5自由基捕捉試驗 65
4.6複合金屬改質生物炭催化CP降解污泥中4-NP 67
4.6.1劑量效應 67
4.6.2初始pH值效應 69
4.6.3反應基質濃度效應 71
4.6.4自由基捕捉試驗 73
第五章 結論與建議 75
5.1結論 75
5.2建議 77
參考文獻 78
附錄一 97
附錄二 101
附錄三 108

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