含氯溶劑大量被使用於工業上金屬及電子零件之清洗及乾洗等作業，當其洩漏至地下水後，無法完全溶解並形成重質非水相液體，其中以三氯乙烯(trichloroethylene, TCE)和四氯乙烯(perchloroethylene, PCE)最為常見。現地化學氧化法為處理受TCE污染之地下水的整治技術之一，其原理是將氧化劑送入到地下，以轉換目標污染物，並降低其質量、移動性及毒性的方法。本研究以高錳酸鉀(KMnO4)氧化劑進行TCE去除，研究分為實驗室及現地試驗兩部分，實驗室試驗包括氧化劑衰減試驗、土壤氧化劑需求量試驗(soil oxygen demand, SOD)、磷酸氫二鈉(Na2HPO4)對二氧化錳(MnO2)之抑制生成試驗、高錳酸鉀批次氧化試驗及管柱試驗等。氧化劑衰減試驗結果顯示高錳酸鉀於自然環境下不易自解，而SOD試驗結果則顯示SOD隨著氧化劑濃度增高呈上升趨勢。在抑制生成試驗結果顯示，隨莫耳濃度比([Na2HPO4]/[KMnO4])增加，磷酸氫二鈉可提升抑制二氧化錳生成率。在高錳酸鉀批次氧化試驗結果顯示，氧化劑濃度越高，其污染物氧化效率有增加之趨勢，且隨反應時間增加，氧化效率逐漸下降；一階動力模擬結果顯示假一階速率常數隨氧化劑濃度上升有升高趨勢，半衰期為24.3-251 min；二階動力模擬結果顯示二階速率常數隨氧化劑濃度上升呈下降趨勢。管柱試驗結果顯示管柱內TCE貫穿體積為5.04-5.06 pore volume(PV)，通入高錳酸鉀能有效氧化TCE污染物，其氧化時間及氧化效率優於以去離子水沖排；另外添加抑制劑磷酸氫二鈉並不會影響TCE之氧化去除效率。本研究之第二階段為現地試驗，研究中挑選某一TCE污染場址進行高錳酸鉀之氧化試驗。研究中所選定之測試區塊共包含八口整治井，其TCE初始濃度及位置分別為上游C1=0.59 mg/L、C1-E=0.64 mg/L、C1-W=0.61 mg/L三口；中游EW-1=0.65 mg/L、EW-1E=0.62 mg/L、EW-1W=0.57 mg/L；下游口C2=0.62 mg/L及C3=0.35 mg/L，每口相鄰監測井距離約為3 m。第一次試驗中於三口注藥井(C1、C1-E、C1-W)注入2,700 L之KMnO4(濃度：5000 mg/L)，於每6小時進行一次灌注，共進行3次注藥，總試驗期程為72小時。注入後除三口注藥井之TCE濃度下降至偵測極限以下(＜0.0025 mg/L)，其餘監測井濃度變化不大。第二次試驗於注藥井EW-1注入2700 L之KMnO4(濃度：5000 mg/L)，於每48小時進行一次灌注，共進行6次注藥，總試驗期程為264小時。注入後注藥井EW-1 TCE濃度降低至偵測極限以下，而監測井(C1、C1-E、C1-W、EW-1E、EW-1W、C2及C3)TCE濃度下降至0.35-0.49 mg/L。顯示以高錳酸鉀氧化劑整治受含氯溶劑污染之地下水具一定成效。造成兩次試驗成效差異之原因為試驗注入頻率及期程不同，且注入位置和受地下水地形之因素，而影響氧化劑傳輸進而造成兩次試驗成效相異。現地試驗後，地下水温度及pH值無太大改變，維持在26-28℃及6-7。導電度及氧化還原電位則有上升趨勢，導電度由500 μS/cm上升至1000 μS/cm，而氧化還原電位則由200 mV上升至600 mV。高錳酸鉀、二氧化錳及總錳濃度於注入井有明顯提升，而總有機碳、鹼度及氯離子數值未有顯著改變。此外，試驗前後各監測井之微水試驗(slug test)結果顯示，試驗前後水力傳導係數維持在10-4-10-5 m/sec，並無顯著變化。此結果顯示現地試驗期間並未顯著影響現地地下水之透水性。

Groundwater at many existing and former industrial sites and disposal areas is contaminated by halogenated organic compounds that were released into the environment. The chlorinated solvent trichloroethylene (TCE) is one of the most ubiquitous of these compounds. In situ chemical oxidation (ISCO) has been successfully used for the removal of TCE. The objective of this study was to apply the ISCO technology to remediate TCE-contaminated groundwater. In this study, potassium permanganate (KMnO4) was used as the oxidant during the ISCO process. The study consisted bench-scale and pilot-scale experiments. In the laboratory experiments, the major controlling factors included oxidant concentrations, effects of soil oxidant demand (SOD) on oxidation efficiency, and addition of dibasic sodium phosphate on the inhibition of production of manganese dioxide (MnO2). Results show that higher molar ratios of KMnO4 to TCE corresponded with higher TCE oxidation rate under the same initial TCE concentration condition. Moreover, higher TCE concentration corresponded with higher TCE oxidation rate under the same molar ratios of KMnO4 to TCE condition. Results reveal that KMnO4 is a more stable and dispersive oxidant, which is able to disperse into the soil materials and react with organic contaminants effectively. Significant amount of MnO2 production can be effectively inhibited with the addition of Na2HPO4. Results show that the increase in the first-order decay rate was observed when the oxidant concentration was increased, and the half-life was approximately 24.3 to 251 min. However, the opposite situation was observed when the second-order decay rate was used to describe the reaction. Results from the column experiment show that the breakthrough volumes were approximately 50.4 to 5.06 pore volume (PV). Injection of KMnO4 would cause the decrease in TCE concentration through oxidation. Results also indicate that the addition of Na2HPO4 would not inhibit the TCE removal rate. In the second part of this study, a TCE-contaminated site was selected for the conduction of pilot-scale study. A total of eight remediation wells were installed for this pilot-scale study. The initial TCE concentrations of the eight wells were as follows: C1 = 0.59 mg/L, C1-E = 0.64 mg/L, C1-W = 0.61 mg/L, EW-1 = 0.65 mg/L, EW-1E = 0.62 mg/L, EW-1W = 0.57 mg/L, C2 = 0.62 mg/L, C3 = 0.35 mg/L. C1, EW-1, C2, and C3 were located along the groundwater flow direction from the upgradient (C1) to the downgradient location (C3), and the distance between each well was 3 m. C1-E and C1-W were located in lateral to C1 with a distance of 3 m to C1. EW-1E and EW-1W were in lateral to EW-1 with a distance of 3 m to EW-1. In the first test, 2,700 L of KMnO4 solution was injected into each of the three injection wells (C1, C1-E, and C1-W) with concentration of 5,000 mg/L. Three injections were performed with an interval of 6 hr between each injection. After injection, the TCE concentrations in those three wells dropped down to below detection limit (<0.0025 mg/L). However, no significant variations in TCE concentrations were observed in other wells. In the second test, 2,700 L of KMnO4 solution was injected into injection well (EW-1) with concentration of 5,000 mg/L. Six injections were performed with an interval of 6 hr between each injection. After injection, the TCE concentrations in the injection well dropped down to below detection limit (<0.0025 mg/L). TCE concentrations in (C1, C1-E, C1-W, EW-1E, EW-1W, C2, and C3) dropped to 0.35-0.49 mg/L. After injection, no significant temperature and pH variation was observed. However, increase in conductivity and oxidation-reduction potential (ORP) was observed. This indicates that the KMnO4 oxidation process is a potential method for TCE-contaminate site remediation. The groundwater conductivity increased from 500 μS/cm to 1,000 μS/cm, and ORP increased from 200 to 600 mv. Increase in KMnO4, MnO2, and total Mn was also observed in wells. Results from the slug tests show that the hydraulic conductivity remained in the range from 10-4 to 10-5 m/sec before and after the KMnO4 injection.

謝誌 I
摘要 III
Abstract V
目錄 IX
表目錄 XIII
圖目錄 XV
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 5
2.1 地下水含氯溶劑化合物之污染來源 5
2.1.1 DNAPLs於地下水之傳輸特性 7
2.1.2 TCE特性及對人體之危害 11
2.2 受含氯溶劑污染之土壤及地下水整治技術 18
2.3 現地化學氧化技術分類及概述 20
2.3.1 氧化劑反應與應用特性 22
2.4 高錳酸鉀特性介紹 26
2.5 高錳酸鉀氧化機制 27
2.6 高錳酸鉀於不同酸鹼環境下之反應 29
第三章 實驗與方法 31
3.1 研究流程 31
3.2 實驗材料及設備 32
3.2.1 實驗藥品 32
3.2.2 實驗器材 33
3.3 研究方法 34
3.3.1 氧化劑去除污染物試驗 34
3.3.2 氧化劑衰減試驗 35
3.3.3 土壤SOD試驗 35
3.3.4 土壤粒徑分析 36
3.3.5 掃描式電子顯微鏡分析(scanning electron microscope, SEM) 36
3.3.6 磷酸氫二鈉對二氧化錳之抑制生成試驗 37
3.3.7 管柱試驗 38
3.4 分析方法 40
3.4.1含氯有機物 40
3.4.2 高錳酸鉀 40
3.4.3 二氧化錳 42
3.4.4 總錳 42
3.4.5 其他水質分析項目 42
3.5 場址介紹 43
3.5.1 場址地形與地勢 44
3.5.2 場址相關背景概述 48
3.5.3 地下水位及流向 50
3.6 現地前置作業 54
3.7 現地化學氧化試驗 63
3.7.1 氧化劑濃度及注藥方式 64
3.7.2 現地操作紀錄 65
3.7.3 現地氧化反應影響因子參數 66
第四章 結果與討論 67
4.1 氧化劑批次試驗 67
4.1.1 氧化劑衰減試驗 67
4.1.2 土壤氧化劑需求&#63870;試驗 70
4.1.3 磷酸氫二鈉對二氧化錳之抑制生成試驗 72
4.1.4 高錳酸鉀氧化批次試驗 75
4.2 管柱污染物去除試驗 82
4.3 管柱試驗土壤表面型態比較 85
4.4 現地試驗成效評估 88
4.4.1 反應溫度對現地氧化之影響 88
4.4.2 pH參數現地影響 89
4.4.3 導電度(EC)與氧化還原電位(ORP) 90
4.4.4 目標污染物濃度趨勢分析 94
4.4.5 地下水中高錳酸鉀與二氧化錳濃度之變化 99
4.4.6 總錳濃度變化 104
4.4.7 總有機碳、鹼度及氯離子 107
4.4.8 水力傳導係數 109
4.5 整治費用評估 111
第五章 結論與建議 113
5.1 結論 113
5.2 建議 115
參考文獻 117

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