臺灣博碩士論文加值系統

由於開放油品進口及加油站民營化，使得油品在儲存及運送活動愈趨頻繁，而加油站的地下輸油管線和地下儲油槽會因埋藏的年代久遠而使滲漏的機會增大。由於燃料油污染土壤及地下水之整治困難度高於受汽油及柴油污染之地下環境，故本研究希望應用Fenton-like氧化技術處理難移除/分解之燃料油，並評估鐵氧礦物、磷酸二氫鉀、界面活性劑以及土壤有機質對Fenton-like處理效率之影響。
研究結果顯示，當燃料油濃度為3%(w/w)時，總石油碳氫化合物(total petroleum hydrocarbons, TPH)之分解率依序為3% H2O2 (84.8%)＞0.05% H2O2 (56.7%)；燃料油濃度為0.5%(w/w)時，TPH分解率依序為6% H2O2 (69.1%)＞3% H2O2 (54.0%) ＞0.05% H2O2 (32.6%)。氧化結果顯示，單純過氧化氫對TPH之氧化能力不如Fenton-like處理程序。而在界面活性劑干擾下，6% H2O2處理0.5 %(w/w)之燃料油污染土時，可容許之界面活性劑濃度為0.7%(w/w)以下。在添加磷酸二氫鉀影響方面，磷酸二氫鉀會抑制水中的亞鐵或鐵氧礦物催化過氧化氫，造成污染物去除效率減低，當添加2.2 mM之KH2PO4時，雖可提高H2O2之穩定性，但TPH分解效率較差。在Fenton-like反應中，pH趨近於6至7，鐵氧礦物溶解量會較少，氫氧自由基之產生大多由鐵氧礦物的固體表面催化所產生。Fenton-like氧化燃料油之副產物判定推測發現不論以3% H2O2處理3%(w/w)燃料油或 6% H2O2處理0.5%(w/w)燃料油，皆有酸類支鏈產生或產生酸類化合物，此結果表示當Fenton或Fenton-like氧化能力不足以破壞化合物結構時，僅有支鏈破壞重組的情況發生，因此產生化合物支鏈改變，但分子量無明顯變化的情況發生。

Soil and groundwater at many existing and former industrial areas and disposal sites is contaminated by petroleum hydrocarbons that were released into the environment. Among those petroleum hydrocarbons, fuel oil is more difficult to treat compared to gasoline and diesel fuel due to its characteristics of low volatility, low biodegradability, and low mobility. Thus, a combination of several different treatment technologies is required to remediate fuel oil contaminated soil or groundwater. The objective of this study was to assess the potential of applying Fenton-like oxidation process to remediate fuel-oil contaminated soils. The following tasks were performed in this study: (1) determination of the optimal oxidation conditions, (2) evaluation of the efficiency of chemical by Fenton-like process after the pretreatment of surfactant flushing, and (3) evaluation of the stability of H2O2 by the addition of potassium dihydrogen phosphate (KH2PO4). Total petroleum hydrocarbons (TPH) in soil were analyzed to determine the effectiveness of the oxidation treatment.
Results from this study show that the highest TPH removal efficiency (84.8%) was obtained for soils containing 3%(w/w) of fuel oil when 3% of H2O2 was applied followed by 0.05% of H2O2 with 56.7% of TPH removal. Results also show that approximately 69.1% of TPH removal was detected with soils containing 5%(w/w) of fuel oil when 6% of H2O2 was applied followed by 3% of H2O2 with 56.7% of TPH removal and 0.05% of H2O2 with 32.6% of TPH removal. Results also indicate that Fenton-like process has much higher oxidation efficiency than using H2O2 alone. The oxidation efficiency was significantly affected when the contaminated soils were pretreated with surfactant. Results reveal that the maximum allowable surfactant addition was approximately 0.7% (w/w) for soils containing 0.5% (w/w) of fuel oil when 6% of H2O2 was applied. Addition of 2.2 mM of potassium dihydrogen phosphate influence could increase the stability of H2O2, but caused the decrease in the efficiency of TPH removal.
During the Fenton-like reaction, pH values were close to 6 to 7. The neutral to slightly acidic conditions caused the decreased dissolution rate of iron minerals. This would also cause the decreased production of hydroxyl radicals from the surface of iron minerals. Results from the byproduct analysis show that the oxidation potential of Fenton-like process is not strong enough to completely destroy the fuel oil to non-toxic end products. The oxidation process produced byproducts containing carboxyl groups with molecular weights similar to their parent compounds.

目 錄
謝 誌 I
摘 要 II
Abstract III
目 錄 IV
表目錄 VI
圖目錄 VII
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 3
2.1 燃料油基本介紹 3
2.2 土壤及地下水油品污染概況 5
2.3 土壤及地下水整治技術發展趨勢 6
2.4 現地化學氧化技術介紹 8
2.5 Fenton-like氧化法技術介紹 12
2.5.1 Fenton 及Fenton-like氧化原理及機制介紹 12
2.5.2 Fenton-like氧化法之優缺點 16
2.5.3 Fenton-like氧化法之影響因子 17
2.5.4 Fenton-like氧化後之副產物 27
2.5.5 Fenton-like氧化反應之•OH生成量推估 29
第三章 材料及方法 31
3.1 實驗材料 31
3.1.1 實驗藥品 31
3.1.2 實驗器材 32
3.2 實驗方法 33
3.2.1土壤基本性質分析 33
3.2.2 人工製備燃料油污染土 35
3.2.3 燃料油污染土之飽和吸附濃度推估 36
3.2.4研究流程 37
3.2.3 Fenton-like氧化試驗 39
3.2.5 燃料油之總石油碳氫化合物分析方法與步驟 42
3.2.6 燃料油氧化後副產物之評估 43
第四章 結果與討論 45
4.1 土壤基本性質分析 45
4.2 燃料油污染土之飽和吸附濃度推估 47
4.3 不同操作條件下Fenton-like氧化燃料油之影響 49
4.3.1 不同過氧化氫濃度 49
4.3.2 去有機質之影響 54
4.3.3 去有機質及去鐵氧礦物之影響 57
4.3.4 添加磷酸氫二鉀之影響 60
4.3.5 界面活性劑濃度之影響 62
4.4 Fenton-like氧化燃料油期間溫度之變化 64
4.5 燃料油氧化反應速率分析 67
4.6 鐵氧化物催化效應之型態推估 70
4.7 燃料油降解趨勢 72
4.8 燃料油氧化後副產物評估 75
第五章 結 論 82
第六章 建 議 84
參考文獻 86

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