臺灣博碩士論文加值系統

本論文以電化學地質氧化系統進行實驗室尺度三氯乙烯污染地下水及現地模場重金屬污染土壤整治之研究，於實驗室尺度，探討Fe/Al氧化電極表面微結構特性及進行三氯乙烯污染地下水整治試驗；再將電化學系統擴大尺度至重金屬污染土壤模場系統，評估重金屬處理效能及土壤鍵結型態對重金屬去除率之影響，同時建立現地本系統之現地標準作業流程 (SOP)。並進行電動力技術經濟成本分析，作為未來將電動力技術廣泛推廣至實場整治之參考依據。
以掃描電子顯微鏡 (SEM) 輔以EDS進行氧化電極表面拍攝及半定量分析，結果顯示金屬Fe之重量百分比介於70.2% ~ 70.7%之間；進一步藉由X-射線繞射進行晶格結構分析，發現於 (0 1 2)、(1 0 4)、(3 1 1)、(0 2 4) 及 (3 0 0) 皆有Fe2O3及Fe3O4之特徵峰值，由此確認Fe/Al氧化電極表面晶格為Fe2O3及Fe3O4。
電化學液相降解TCE試驗中，研究結果發現，於施加3.0 V/cm電位坡降、pH = 3.0環境下，分別添加10.0 mM SPS、12.0 mM PMS及2.0 mM KMnO4氧化劑，10.0 mM SPS及2.0 mM KMnO4氧化劑分別於整治5.0小時及3.0小時後達降解率99.9%以上，添加12.0 mM PMS氧化劑，於整治7.0小時後降解率達69.9%；進一步比較後發現，KMnO4氧化劑降解TCE僅3.0小時即達降解率99.9%，具最佳整治成效，因KMnO4氧化劑不經催化即有55.4%之整治效益，相較分別單獨添加SPS及PMS氧化劑，整治成效僅分別為10.3%及8.8%，SPS及PMS氧化劑較具長時間之電化學催化優勢，其中又以SPS氧化處理TCE成效較佳。
現地模場重金屬污染土壤整治試驗中，已建立電動力系統模場設置標準作業流程 (SOP)。整治試驗分別於蜂巢型及方型排列模組之陽、陰極端使用Al電極，施加0.6 V/cm之電位坡降、以地下水作為操作流質 (Test C1及D1)，重金屬Cu、Zn、Cr、Ni及Pb去除率分別介於-6.6% ~ 43.7%；提高電位坡降至1.0 V/cm (Test C2及D2)，重金屬離子去除率分別介於-24.8% ~ 6.1%，因受陰極井端釋出之氫氧根離子影響，整治成效下降；更換陽極端由Al惰性電極至Fe/Al氧化電極 (Test C3及D3)，重金屬離子去除率分別介於1.5% ~ 31.9%，使用Fe/Al氧化電極作為陽極端電極，使土壤重金屬由強鍵結態轉化至弱鍵結態後移除；另更換由地下水至0.05 M乳酸 (Test C4及D4)，重金屬離子去除率分別介於-23.4% ~ 24.5%，蜂巢型排列模組因電流密度變化趨勢較大致整治成效較方型排列模組高；分別再提升電位坡降及乳酸濃度至1.4 V/cm及0.30 M (Test C5及D5)，重金屬離子去除率分別介於-30.1% ~ 39.4%，因實驗期間之降雨使乳酸受到稀釋而導致整治成效下降。
蜂巢型及方型排列模組於電動力試驗整治前弱鍵結型態比例分別介於0.0% ~ 14.2%及0.0% ~ 4.3%之間，研究結果發現，提升電位坡降及更換操作流質由地下水至乳酸，重金屬弱鍵結型態部分被移除，但陽極端電極更換至Fe/Al氧化電極後發現其最具弱鍵結型態轉化效益，蜂巢型及方型排列模組弱鍵結型態比例分別由0.0% ~ 12.4%及0.0% ~ 12.8%提升至13.2% ~ 19.2%及0.0% ~ 23.2%之間。
本論文經濟成本於實驗室尺度三氯乙烯污染地下水整治試驗中，處理成本約介於140.0 NTD/m3 ~ 97,740 NTD/m3之間，僅約Christopher (2009) 執行電動力技術成本之5.2% ~ 84.1%；現地模場重金屬污染土壤整治試驗中，處理成本約介於1,140.6 NTD/m3 ~ 9,701.8 NTD/m3之間，僅約Christopher (2009) 執行電動力技術成本之33.1% ~ 80.8%，顯示本研究具經濟優勢。

This study is focus on the remediation of Trichloroethylene (TCE) contaminated groundwater at lab-scale and heavy metal contaminated soil in the field site by ElectroChemical Geooxidation (ECGO) system. On a lab-scale, the surface microstructure characteristics of Fe/Al oxidation electrodes are investigated in remediation experiments for TCE contaminated groundwater. The ECGO system was expanded to the heavy metal contaminated soil field system to evaluate the effect of heavy metal treatment efficiency and soil bonding on the removal rate of heavy metals, and at the same time, a Standard Operating Procedure (SOP) of ECGO system is established. After completing the test, an analysis of the technical and economic cost of electric power technology will be carried out as a reference for the extensive promotion of electric power technology to the field renovation in the future.
The surface imaging and semi-quantitative analysis of the Fe/Al oxidation electrode are investigated by Scanning Electron Microscope (SEM) and EDS. Results showed that 70.2% ~ 70.7% of iron is coated on the electrode surface. The lattice structure was further analyzed by X-Ray Diffraction. The characteristic peak of Fe2O3 and Fe3O4 at (0 1 2), (1 0 4), (3 1 1), (0 2 4) and (3 0 0) are found, which confirms the surface lattice of iron are Fe2O3 and Fe3O4.
For TCE degradation in aqueous phase, the results found under an environment of 3.0 V/cm potential gradient and pH = 3.0, 10.0 mM SPS, 12.0 mM PMS and 2.0 mM KMnO4 oxidants, 10.0 mM SPS and 2.0 mM KMnO4 oxidants were added respectively. The degradation rate of SPS and KMnO4 oxidant reached more than 99.9% after 5.0 hours and 3.0 hours of remediation, and the degradation rate of PMS oxidants reached 69.9% after 7.0 hours of remediation. After further comparison, it was found that KMnO4 oxidant degraded TCE in only 3.0 hours. The rate of 99.9%, with the best remediation effect, because the KMnO4 oxidant has 55.4% remediation efficiency without catalysis. Compared with adding SPS and PMS oxidants separately, the remediation effect is only 10.3% and 8.8%, respectively. SPS and PMS oxidants are more effective. It has the advantages of long-term electrochemical catalysis. Among them, the effect of SPS oxidation treatment TCE is better.
A Standard Operating Procedure (SOP) of ECGO system in heavy metal contaminated site is established. For the model field setting of the electric power system has been established. The Al electrodes were used on the anode and cathode well of the honeycomb and square modules, applies a potential gradient of 0.6 V/cm, processing fluid was setting for groundwater (Test C1 and D1), the efficiency of heavy metals Cu, Zn, Cr, Ni and Pb is between -6.6% ~ 43.7%; increase of the potential gradient to 1.0 V/cm (Test C2 and D2), the removal rate of heavy metal are between -24.8% ~ 6.1%, due to the hydroxide ions were produced at the cathode well, reduce the effect of heavy metal remediation. The anode well is replaced from Al inert electrode to Fe/Al oxidation electrode (Test C3 and D3). The removal rate of heavy metal is between 1.5% ~ 31.9%. The Fe/Al oxidation electrode is used as the anode electrode to remove the heavy metals from strong bonding to weak bonding; the other is replaced from groundwater to 0.05 M lactic acid (Test C4 and D4), and the removal rate of heavy metals is between -23.4% ~ 24.5%, the honeycomb module has a higher remediation effect than the square module due to the greater change in current density; the potential gradient and the lactic acid concentration were increased to 1.4 V/cm and 0.30 M (Test C5 and D5), heavy metals removal rate was between -30.1% ~ 39.4%, and the lactic acid was diluted by the rainfall during the experiment, which led to a decrease in the treatment effect.
In the honeycomb and square module, the weak bonding of metals before ECGO experiments is in the range of 0.0% ~ 14.2% and 0.0% ~ 4.3%, respectively. Before the ECGO remediation, increase potential gradient and replace processing fluid from groundwater to lactic acid, the weak bonding are partially removed, but the anode electrode is replaced with Fe/Al oxidation electrode and found to have the weak bonding efficiency of form transformation, the proportion of weak bonding forms of honeycomb and square modules has been increased from 0.0% ~ 12.4% and 0.0% ~ 12.8% to 13.2% ~ 19.2% and 0.0% ~ 23.2%, respectively.
The treatment cost of TCE contaminated groundwater in this study is in the range of 140.0 NTD/m3 ~ 97,740 NTD/m3, which is only about 5.2% ~ 84.1% of Christopher (2009); furthermore, the treatment cost of heavy metal contaminated soil in the study is the range of 1,140.6 NTD/m3 ~ 9,701.8 NTD/m3, which is only about 33.1% ~ 80.8% of the cost of Christopher (2009). The result showed the ECGO technology is a practical technology for remediation of Chloride organic compounds and heavy metals with economic insensitive.

目錄 II
表目錄 X
圖目錄 XIII
摘要 1
ABSTRACT 3
第一章 前言 6
1.1研究緣起 6
1.2研究目的 9
1.3研究內容 9
第二章 文獻回顧 11
2.1含氯有機污染物來源及用途 11
2.2含氯有機污染物之特性及流佈 13
2.2.1三氯乙烯之物化特性 14
2.2.2三氯乙烯對環境及人體健康之影響 14
2.2.3三氯乙烯之環境/職業暴露因子 19
2.2.3.1環境暴露 19
2.2.3.2職業暴露 23
2.3含氯有機物整治技術 24
2.3.1物理處理 24
2.3.2生物處理 27
2.3.3高級氧化處理 29
2.3.3.1羥基自由基氧化機制 30
2.3.3.2過硫酸鹽氧化機制 33
2.3.3.3過錳酸鉀氧化機制 37
2.4含氯有機物之降解途徑 38
2.4.1還原脫氯 38
2.4.2共代謝 38
2.5環境關心之重金屬污染物 40
2.5.1重金屬污染物基本物化特性及其管制標準 40
2.5.2土壤重金屬之結合型態 44
2.6管制重金屬來源及流佈 48
2.6.1管制重金屬流佈 48
2.6.2管制重金屬對環境及人體健康之影響 52
2.7重金屬污染土壤整治技術 53
2.7.1土壤沖洗 (Soil Flushing) 53
2.7.2土壤淋洗 (Soil Washing) 58
2.7.3玻璃化法 (Vitrification) 59
2.7.4植生復育 (Phytoremediation) 60
2.7.5化學固化 (Chemical Immobilization) 61
2.8電化學地質氧化技術原理與機制 62
2.8.1處理機制 64
2.8.2電動力技術之影響因子 71
2.8.2.1 pH環境影響因子 71
2.8.2.2土壤成分影響因子 72
2.8.2.3電極材料影響因子 73
2.8.2.4電壓/電流影響因子 74
2.8.2.5共溶劑影響因子 75
2.8.2.6電極排列影響因子 75
2.9電動力技術應用於污染處理之研究 78
2.9.1實驗室尺度 78
2.9.2實場尺度 80
2.10電動力結合其他技術整治成效 82
2.10.1電動力結合植生復育法整治成效 83
2.10.2電動力結合化學氧化法整治成效 84
2.10.3電動力結合滲透性反應牆整治成效 86
第三章 研究方法 88
3.1研究架構 88
3.2實驗設備與材料 88
3.2.1儀器與設備 88
3.2.2實驗材料 90
3.3含氯有機物分析 92
3.3.1前處理 92
3.3.1.1低懸浮微粒 (LSS) 92
3.3.1.2高懸浮微粒 (HSS) 93
3.3.2氣相層析分析方法 93
3.4重金屬分析 94
3.4.1前處理 94
3.4.2土壤型態分析 (序列萃取) 94
3.4.3感應耦合電漿發射光譜儀 (ICP-OES) 分析方法 96
3.5 Fe/Al氧化電極製備及分析 96
3.5.1製備方法 96
3.5.1.1實驗室尺度電極 97
3.5.1.2實場尺度電極 98
3.5.2電極塗佈量分析 98
3.5.2.1實驗室尺度電極 99
3.5.2.2實場尺度電極 99
3.5.3電極之鐵型態分析 100
3.5.3.1總鐵分析 100
3.5.3.2亞鐵分析 100
3.6實驗室尺度三氯乙烯液相降解整治試驗 101
3.7電動力現地模組系統設計 103
3.7.1前置工程施作階段 103
3.7.2整治作業階段 104
3.7.3場址復原階段 105
3.8實場尺度重金屬污染土壤整治試驗 106
3.8.1試驗模場背景特性分析 106
3.8.2土壤採樣作業 108
3.8.3蜂巢型排列模組 108
3.8.4方型排列模組 108
3.9土壤基本性質分析 109
3.9.1土壤含水率 109
3.9.2土壤陽離子交換容量 (CEC) 110
3.9.3土壤pH值 110
3.9.4土壤有機質 111
3.9.5土壤界達電位 111
3.9.6土壤比表面積測定 112
3.10實驗室之品保/品管 112
第四章 結果與討論 114
4.1土壤基本特性 114
4.2 Fe/Al氧化電極塗佈量及特性分析 114
4.2.1電極塗佈量 116
4.2.2電極表面特性 117
4.2.2.1掃描電子顯微鏡/能量色散X-射線光譜分析 (SEM/EDS) 117
4.2.2.2 X-射線繞射分析 (XRD) 118
4.3實驗室尺度電化學液相降解TCE及其副產物分析 120
4.3.1過硫酸鈉 (Sodium Persulfate, SPS) 系統 120
4.3.1.1實驗結果及分析 122
4.3.1.2副產物分析 126
4.3.1.3降解動力學分析 130
4.3.2過一硫酸氫鉀 (PMS) 系統 132
4.3.2.1實驗結果及分析 135
4.3.2.2副產物分析 139
4.3.2.3降解動力學分析 143
4.3.3過錳酸鉀 (KMnO4) 系統 146
4.3.3.1實驗結果及分析 146
4.3.3.2副產物分析 150
4.3.3.3降解動力學分析 154
4.3.4氯離子及碳原子質量平衡 154
4.3.4.1氯離子分析 157
4.3.4.2碳原子分析 160
4.3.5小結 164
4.4電動力現地模場系統設計 168
4.4.1前置工程施作階段 168
4.4.1.1選址、現場勘查及地主整治意願評估 169
4.4.1.2土壤 (土壤污染場址) 或地下水污染 (地下水污染場址) 調查作業 170
4.4.1.3電動力技術適宜性評估 172
4.4.1.4電極排列模組設計及規劃 172
4.4.1.5地電阻測勘及整流器設計/製造 173
4.4.1.6整地及電極井設置作業 181
4.4.1.7電極安裝及架設 183
4.4.1.8電力系統架設/測試 184
4.4.2整治作業階段 187
4.4.2.1電動力技術整治 187
4.4.2.2電動力相關整治數值觀測/監測 187
4.4.2.3採樣作業 187
4.4.2.4電力系統維護 188
4.4.2.5數據分析及彙整 188
4.4.2.6整治成效及退場時機評估 189
4.4.3場址復原階段 189
4.5現地模場重金屬污染土壤整治試驗 189
4.5.1蜂巢型排列模組 190
4.5.1.1電流密度變化 191
4.5.1.2重金屬殘留濃度分佈 201
4.5.1.3重金屬處理效能分析 340
4.5.2方型排列模組 346
4.5.2.1電流密度變化 347
4.6.2.2重金屬殘留濃度分佈 358
4.5.2.3重金屬處理效能分析 495
4.5.3土壤重金屬鍵結型態分析 502
4.5.3.1蜂巢型排列模組 502
4.5.3.2方型排列模組 523
4.6經濟效益評估 544
4.6.1實驗室尺度三氯乙烯污染地下水 544
4.6.2實場尺度重金屬污染土壤 553
4.6.2.1前置工程施作階段及場址復原階段 553
4.6.2.2整治作業階段 556
4.6.2.3總整治成本分析 563
4.6.3與現行整治技術經濟效益比較 565
第五章 結論與建議 569
5.1結論 569
5.2建議 573
參考文獻 574

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