本研究以三氯乙烯(TCE)作為水溶液及土壤污染整治試驗之標的污染物，並探討採用乳化奈米鐵漿液與電動力法組合技術之整治成效。首先於實驗室利用化學還原法以工業級藥品製備奈米級零價鐵，經X-光繞射分析證實為鐵元素與鐵氧化物，而掃描式電子顯微鏡觀測得奈米鐵粒徑分佈介於30~50 nm間。
大豆油乳液之穩定性探討係使用六種非離子型界面活性劑搭配大豆沙拉油作探討，結果顯示使用混合界面活性劑(Span 80與Tween 40)搭配大豆油之乳化漿液有較佳的乳液穩定性。確定最佳大豆油乳液製備方法後，即結合奈米級零價鐵水溶液、食品級大豆油(Soybean oil)及混合界面活性劑，經充分攪拌，製備得乳化奈米級零價鐵漿液。
對於乳化奈米鐵漿液去除水溶液中三氯乙烯降解之影響，首先，探討乳化奈米級零價鐵漿液之鐵與油相劑量之影響，發現經乳化改質後之奈米鐵確實可提高降解TCE之成效，且奈米鐵劑量在0.75 iron-g/L即可降解TCE(初始濃度10 mg/L)達55 %，而增加油相可改善乳液穩定性，但此對降解TCE之成效卻有負面影響。不同操作變因(pH值、TCE初始濃度、震盪強度)對於TCE降解有不同程度的影響，實驗結果顯示在pH = 6時，可降解TCE濃度達94 %；而較高的TCE初始濃度則有較高的TCE去除率；在未震盪(0 rpm)與外加水平震盪(160 rpm)下，顯示外加動力震盪有較佳降解成效。此外，使用人工配製TCE污染地下水樣，進行乳化奈米級零價鐵處理TCE污染地下水樣，結果顯示地下水中之硝酸鹽與碳酸鹽會抑制零價鐵對TCE的反應性，尤其大量碳酸鹽於反應系統，可能會在鐵表面生成鈍化膜或沉澱。
本研究更進一步利用乳化奈米鐵漿液-電動力法組合技術處理水平土壤管柱系統中的三氯乙烯(98~118 mg/kg)。採用電位梯度為1 V/cm，每天注入定量乳化奈米鐵漿液20 mL(鐵濃度為0.75 g/L)於選定之電極槽內；實驗結果顯示，將乳化奈米鐵漿液注入陽極槽，在強酸且氧化態的環境中，造成鐵迅速腐蝕而耗盡，影響整體降解效果；而乳化奈米鐵漿液注入陰極槽之實驗組，其土壤中三氯乙烯殘存率為33.55 %，且乳化奈米鐵漿液於陰極槽有助於將移出土體的三氯乙烯進行破壞降解，顯示在陰極槽加入乳化奈米鐵漿液有最大的土體中三氯乙烯去除率。

The objective of this research was to evaluate the treatment efficiency of a trichloroethylene(TCE)-contaminated aqueous solution and soil by combined technologies of the emulsified nanoscale zero-valent iron slurry (ENZVIS) and electrokinetic remediation process. Nanoiron was synthesized using the chemical reduction method by industrial grade chemicals. The synthesized nanoparticles contained elemental iron and iron oxide as determined by X-ray diffractmetry(XRD). Micrographs of FE-SEM have shown that a majority of nanoiron were in the size range of 30~50 nm.
The stability study of food-grade soybean oil emulsion was conducted using six non-ionic surfactants and soybean oil. The results have shown that the emulsion prepared by mixed surfactants (Span 80 and Tween 40) and soybean oil yielded a better emulsion stability. Based on the above finding, the nanoiron slurry, soybean oil and aforementioned, mixed surfactants were used to prepare ENZVIS.
Degradation of TCE by ENZVIS under various operating parameters was carried out in batch experiments. The experimental results have indicated that emulsified nanoiron outperformed nanoiron in TCE dechlorination rate. ENZVIS (0.75 g-Fe0/L) degradated TCE (initial conc.= 10 mg/L) down to 45 %. An increase of the oil dosage could improve the stability of the emulsion, but yielding a negative influence on degradation of TCE. Experimental results also showed that ENZVIS could remove TCE up to 94 % when pH=6. It was also formed that a higher TCE initial concentration would result in a higher TCE removal efficiency. In addition, using ENZVIS to degraded TCE-contaminated artificial groundwater has indicated that nitrate and carbonate of groundwater will suppress nanoiron reaction with TCE. Especially, a high concentration of carbonate in the reaction system might form a passive film or precipitates on nanoiron surface.
This study further evaluated the treatment efficiency of combining ENZVIS and electrokinetic technology in treating a TCE-contaminated soil. Experimental conditions were given as follows:(1) initial TCE concentration in the range of 98~118 mg/kg; (2) an electric potential gradient of 1 V/cm; (3) a daily addition of 20 mL ENZVIS; and (4) a reaction time of 10 days. Experimental results have shown that an addition of ENZVIS to the anode reservoir of strongly acidic and oxidative environment would cause nanoiron to corrode rapidly and decrease TCE removal efficiency. On the other hand, an addition of ENZVIS to the cathode reservoir would enhance the degradation of TCE therein. In summary, an addition of ENZVIS to the cathod reservoir would yield the best TCE removal efficiency.

頁碼
聲明切結書 i
謝誌 ii
摘要 iii
Abstract iv
目錄 v
表目錄 ix
圖目錄 x
照片目錄 xii
第一章 前言 1
1.1 研究緣起 1
1.2 研究目的 3
1.3 研究內容 3
第二章 文獻回顧 6
2.1 三氯乙烯之性質與對人體的危害性 6
2.1.1 三氯乙烯之物化性質 6
2.1.2 三氯乙烯對人體的危害性 9
2.2 土壤與地下水受含氯有機物污染之相關整治技術 12
2.2.1 物理/化學處理整理技術 13
2.2.2 生物處理整治技術 14
2.3 零價鐵 18
2.3.1 零價鐵之應用原理 18
2.3.2 影響零價鐵還原脫氯之相關因子 21
2.3.3 三氯乙烯還原脫氯之反應途徑 26
2.4 奈米級零價鐵之發展 29
2.4.1 奈米科技 29
2.4.2 奈米級零價鐵之製備與整治污染物相關研究 29
2.4.3 奈米雙金屬之發展 33
2.4.4 奈米雙金屬整治污染物之相關研究 34
2.4.5 奈米級零價鐵表面改質 36
2.5 界面活性劑 39
2.5.1 界面活性劑簡介 39
2.5.2 非離子型界面活性劑 41
2.5.3 HLB值 42
2.5.4 乳化 43
2.6 電動力法 45
2.6.1 電動力法之傳輸與相關反應機制 45
2.6.2 影響電動力法之相關因子 48
2.6.3 電動力法整治污染物相關研究 49
第三章 實驗材料與方法 51
3.1 實驗材料 51
3.1.1 奈米級零價鐵製備 51
3.1.2 乳化奈米級零價鐵漿液之製備 52
3.1.3 土壤樣品來源與前處理 52
3.1.4 其它試藥及材料 52
3.2 實驗設備 55
3.2.1 儀器設備 55
3.2.2 電動力技術管柱處理系統 57
3.3 奈米級零價鐵基本性質分析 59
3.3.1 X-光繞射(X-Ray Diffraction, XRD)分析 59
3.3.2 掃描式電子顯微鏡(Scanning Electron Microscope, SEM)分析 59
3.3.3 掃描式電子顯微鏡-X-光能譜分析儀(SEM-EDS)與能量分佈面 掃描(EDS-Mapping)分析 60
3.3.4 動態光散射(Dynamic Light Scattering, DLS)分析 60
3.4 大豆油乳液穩定性探討 62
3.4.1 選擇適當HLB值 62
3.4.2 選擇適當混合界面活性劑 63
3.4.3 不同添加順序 63
3.5 乳化奈米級零價鐵漿液去除三氯乙烯水溶液試樣之批次實驗 63
3.5.1 乳化奈米級零價鐵漿液之微胞觀測 64
3.5.2 三氯乙烯水溶液批次試驗相關分析與試樣製備 64
3.5.3 油/水對TCE分配係數批次實驗 66
3.5.4 儀器分析與操作條件 66
3.6 乳化奈米級零價鐵去除三氯乙烯污染地下水樣 68
3.7 乳化奈米級零價鐵-電動力法去除土壤中三氯乙烯試驗 69
3.7.1 土壤樣品基本性質分析 69
3.7.1.1 粒徑分佈 69
3.7.1.2 比重 70
3.7.1.3 pH值 71
3.7.1.4 含水份 71
3.7.1.5 有機物質含量 72
3.7.1.6 灼燒減量 72
3.7.1.7 陽離子交換容量 72
3.7.2 人工污染土樣製備與管柱裝填 73
3.7.3 土樣反應前後分析項目 74
3.7.4 反應過程分析 75
3.7.5 乳化奈米鐵漿液最佳注入位置探討 76
第四章 結果與討論 77
4.1 奈米級零價鐵基本性質分析 77
4.1.1 X-光繞射(X-Ray Diffraction, XRD)分析 77
4.1.2 場發射型掃描式電子顯微鏡(FE-SEM)分析 79
4.1.3 掃描式電子顯微鏡-X-光能譜分析儀(SEM-EDS)與能量分佈面 掃描(EDS-Mapping)分析 80
4.1.4 動態光散射(Dynamic Light Scattering, DLS)分析 83
4.2 大豆油乳液穩定性探討 84
4.2.1 選擇適當HLB值 84
4.2.2 選擇適當混合界面活性劑 86
4.2.3 不同添加順序 86
4.3 乳化奈米級零價鐵漿液去除三氯乙烯水溶液試樣之批次實驗 88
4.3.1 乳化奈米級零價鐵漿液之製備與微胞觀測 88
4.3.2 前導實驗-乳化奈米級零價鐵漿液之鐵與油相劑量 90
4.3.3 油/水對TCE之分配係數批次實驗 95
4.3.4 不同操作變因對降解三氯乙烯之影響 96
4.4 乳化奈米級零價鐵去除三氯乙烯污染地下水樣 106
4.5 乳化奈米級零價鐵─電動力法去除土壤中三氯乙烯試驗 108
4.5.1 土壤樣品基本性質分析 108
4.5.2 標的污染物 110
4.5.3 乳化奈米鐵漿液最佳注入位置探討 111
第五章 結論與建議 120
5.1 結論 120
5.2 建議 123
參考文獻 124
附錄 139
附表1 不同溫度下的水之相對密度及校正因子K值 139
附表2 台灣糖業-大豆沙拉油脂肪酸組成表 140
附表3 圖4-6 不同奈米鐵劑量之乳化鐵漿液去除水溶液中TCE之情形 實驗數據 141
附表4 圖4-7 不同反應系統對TCE之降解成效比較實驗數據 141
附表5 圖4-8 不同油相劑量之乳化鐵對TCE降解成效之影響實驗數據 142
附表6 圖4-13 乳化鐵在不同初始pH值下對於三氯乙烯之降解成效 比較實驗數據 142
附表7 圖4-17 不同三氯乙烯初始濃度對其降解成效之影響實驗數據 143
附表8 圖4-18有無震盪對降解三氯乙烯之影響實驗數據 143
附表9 圖4-19 乳化奈米鐵降解TCE污染去離子水樣與模擬地下水樣 比較實驗數據 144
附表10 圖4-23 土壤管柱槽液pH值隨處理時間變化圖實驗數據 144
附表11 圖4-24 陰極槽累積電滲透流流量隨處理時間變化圖實驗數據 145
附表12 圖4-25 操作電流隨處理時間變化圖實驗數據 145
附表13 圖4-26 陰極槽內三氯乙烯含量隨處理時間變化圖實驗數據 146
附表14 圖4-27 陽極槽內三氯乙烯含量隨處理時間變化圖實驗數據 146
附表15 圖4-28 反應後土壤管柱內殘餘之三氯乙烯含量分佈圖 實驗數據 147
附表16 圖4-29 反應後土壤管柱內土壤pH值分佈圖實驗數據 147
碩士在學期間發表之學術論文 148

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