含氯有機溶劑常被廣泛應用於脫脂、電子零件清洗及乾洗等工業製程中，其中以三氯乙烯(trichloroethylene, TCE)及四氯乙烯(tetrachloroethene, PCE)為國內外最具代表性之含氯有機溶劑。在土壤與地下水中為常見的污染物，且在地下水中因其特性而常以比水重之非水相液體(dense non-aqueous phase liquid, DNAPL)存在難以整治。本研究成功研發一種可緩慢釋放碳源及營養物質，用以提升受TCE污染之地下水生物降解效率，而緩慢釋碳基質其中成分包含大豆油(慢速分解基質)、乳酸鹽(快速分解基質)、生物可分解界面活性劑(Simple Green及卵磷脂)以及維他命，經乳化後可達90%以上乳化效果，且較易擴散於土壤孔隙間，並且能長時間提供微生物行厭氧還原脫氯所需之碳及營養物質。本研究利用自行研發乳化型釋碳基質灌注於南台灣一主要受TCE污染之場址，並結合生物透水性整治牆的概念，加強本場址內TCE生物還原脫氯作用，以防止污染源向下游傳輸擴散。由監測井之採樣分析結果可知，本場址之TCE濃度介於0.03-0.10 mg/L之間。由污染量及水文等相關資料之評估，在上游設置三口井(BW1-1、BW1-1e及BW1-1w)分別直接灌注40 L基質方式做為整治之用，下游設置三口井(C029、C029e及C029w)做為成效評估之用。由地質化學反應得知，溶氧低於0.5 mg/L及氧化還原電位呈現還原態，本研究注入之乳化型釋碳基質可持續緩慢釋出碳源及營養物質，此外厭氧生物反應最終伴隨甲烷化反應，甲烷濃度有上升趨勢，以及醋酸濃度上升且未累積，證實模場中地下水環境呈現厭氧還原狀態。總菌數部分，注入井BW1-1之總菌數以及其餘監測井C029、C029e及C029w之總菌數皆有增加，由此可知乳化型釋碳基質確實可促進微生物生長，使地下水注入區下游地區總菌數呈現增加趨勢。模場試驗結果顯示注入乳化型釋碳基質，上游三口監測井(BW1-1、BW1-1e及BW1-1w)之TCE濃度降解效率分別為93.8%、86.7%及6.25%，監測結果亦顯示於注入後之第五天開始下游監測井測得TCE被微生物分解之副產物順1,2-二氯乙烯(cis1,2-DCE, cDCE)及氯乙烯(vinyl chloride, VC)，其濃度分別為0.002-0.010 mg/L及0.2-0.5 mg/L。並藉由菌相分析法偵測結果可知，現地具有Ralstonia sp.、Clostridium sp.、Uncultured Burkholderiales bacterium、Hydrogenophaga sp.、Acidovorax sp.、Zoogloea sp.、Hydrocarboniphaga sp.、Uncultured Curvibacter sp.、Pseudomonas sp.、Comamonas sp.、Aquabacterium sp.、Variovorax strains等具有降解含氯有機物效果之菌種。由微水試驗結果可知，上游各井注入基質前後透水係數差異甚小，顯示現地添加乳化型釋碳基質，並未造成現場地下水井阻塞。以成本評估模式評估一年的經費為USD13,442 (約NTD389,818)，單位處理費用為173.62 USD/m3。顯示本研究自行配製之乳化型釋碳基質為良好緩釋性物質，且具有長時效供應現地微生物生長之營養鹽降解目標污染物，並符合綠色整治減少二次污染，本研究之效果以提供未來相關整治場址之參考依據。

Soil and groundwater at many existing and former industrial areas and disposal sites is contaminated by halogenated organic compounds that were released into the environment. Halogenated organic compounds are heavier than water. When they are released into the subsurface, they tend to adsorb onto the soils and cause the appearance of DNAPL (dense-non-aqueous phase liquid) pool. Among those halogenated organic compounds, trichloroethylene (TCE), a human carcinogen, is one of the commonly observed contaminants in groundwater. Thus, TCE was used as the target compound in this study. The objective of this study was to develop the emulsified carbon-releasing substrate and apply it as the filling material in the permeable reactive barrier to remediate TCE-contaminated groundwater. In this study, the developed emulsified carbon-releasing substrate contained soybean oil, lactate, biodegradable surfactant (Simple GreenTM and lecithin), and nutrients. Results of emulsion test show that up to 90% of the emulsified carbon-releasing substrate was distributed effectively in the soil pores. The emulsified carbon-releasing substrate was able to provide carbon for the enhancement of in situ anaerobic biodegradation for a long period of time. A pilot-scale study was operated at a TCE-contaminated site located in southern Taiwan. Emulsified carbon-releasing substrate emulsion was pressure-injected into the remediation wells. A total of 120 L of emulsified carbon-releasing substrate was injected into the test site. Based on the groundwater analytical results, dissolved oxygen, oxidation-reduction potential, and sulfate concentrations decreased after injection. However, the anaerobic degradation byproduct, acetic acid, increased after injection. Results also show that the total viable bacteria increased in the upgradient injection (remediation) well. Decrease in TCE concentration (dropped to below 0.01 mg/L) was also observed after substrate injection, and TCE degradation byproducts, cis-1,2-dichloroethene (cDCE) and vinyl chloride (VC) were also observed. Result of microbial analyses show that various TCE-degrading bacteria exist in the groundwater samples including Ralstonia sp., Clostridium sp., Uncultured Burkholderiales bacterium, Hydrogenophaga sp., Acidovorax sp., Zoogloea sp., Hydrocarboniphaga sp., Uncultured Curvibacter sp., Pseudomonas sp., Comamonas sp., Aquabacterium sp., and Variovorax strains. This reveals that the anaerobic dechlorination of TCE is a feasible technology at this site. Slug test result show that only a slight variation in soil permeability of the injection well was observed. This indicates that the substrate injection would not cause clogging of the soil pores. Results from the cost analysis show that the total cost for the test site remediation was approximately USD13,442 per year. This indicates that the developed system has the potential to be developed into an environmentally, economically, and naturally acceptable remedial technology. Knowledge obtained from this study will aid in designing a carbon-released substrate biobarrier system for site remediation.

謝誌 i
摘要 ii
Abstract iv
目錄 vi
圖目錄 viii
表目錄 x
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 土壤及地下水氯化碳氫化合物污染概況 3
2.1.1 含氯碳氫化合物污染概述 3
2.1.2 三氯乙烯之性質及管制標準 6
2.1.3 三氯乙烯之傳輸 10
2.2土壤與地下水整治技術發展趨勢 15
2.2.1 地下水生物整治技術 16
2.2.2 綠色整治技術 20
2.3 三氯乙烯生物反應機制 22
2.3.1 三氯乙烯好氧共代謝反應機制 22
2.3.2 三氯乙烯厭氧還原脫氯反應機制 26
2.4乳化型基質加強生物之整治牆 28
2.5利用乳化型釋碳基質做為厭氧還原脫氯作用之類似場址研究 32
第三章 研究方法、材料與架構 35
3.1 實驗架構 35
3.2 材料與方法 36
3.2.1 藥品材料 36
3.2.2 實驗設備 36
3.3 乳化型釋碳基質之合成 37
3.4 現地場址背景介紹 39
3.5 現地模場試驗 47
3.5.1 水文地質調查 47
3.5.2 現場作業及採樣方式 50
3.6 分析方法 51
3.6.1 污染物分析方法 51
3.6.2 水質分析方法 51
3.6.3 菌相分析方法 54
3.7 Mann-Kendall 模式 57
3.8 成本模式 59
第四章 結果與討論 61
4.1 生物復育現地場址指標性參數變化 61
4.2 電子接受者及供給者分析 65
4.3 三氯乙烯及副產物降解趨勢分析 77
4.4 菌相分析法偵測結果 82
4.5水力傳導係數 94
4.6 整治費用評估 96
第五章 結論與建議 99
5.1 結論 99
5.2 建議 101
參考文獻 103

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