土壤及地下水的污染場址中，含氯脂肪碳氫化合物為常見之重質非水相溶液(dense non-aqueous phase liquids, DNAPLs)污染物，尤以三氯乙烯(trichloroethylene, TCE)最具代表性。由於受DNAPL污染場址之整治是屬於長期性的工作，因此結合加強式厭氧生物整治及基質緩釋機制乃成為現今眾多整治技術中較佳之整治方案。研究第一部份係以過去實驗團隊所研發之長效型膠體基質進行現地模場試驗，其注藥井(RW)於注藥初期能提高其總有機碳含量為1,126 mg/L(背景值為1.901 mg/L)，並能迅速吸附污染物，TCE濃度由背景值0.068 mg/L降至0.022 mg/L，其值低於管制標準(0.050 mg/L)以下，並於研究第350天後，降解率達93%，符合監測標準(0.025 mg/L)，且其酸鹼值趨於穩定並維持厭氧還原態環境。於注藥後第126天後，研究以分子生物技術分析現地相關菌群變化，發現明顯增加之菌群包含可降解含氯有機物之Enterobacter、與脫鹵球菌共生之甲烷菌屬及能生成乙酸及丙酸，並促進脫鹵球菌生長之異營性細菌等，證實本基質能於實場避免水體酸化，達酸鹼緩衝及異味控制之成效，刺激現地相關脫氯菌群生長並降解TCE。研究第二部分以草木灰及改質稻殼灰分別與自製乳化基質進行合成改良，製備具有酸鹼緩衝能力及緩釋碳源之綠色基質，由微生態批次試驗進行60天的結果顯示，添加草木灰之組別，能於初期提供鹼度，以中和發酵所產生之有機酸等酸化問題，其TCE降解率可達82.4%及84.1%。而添加改質稻殼灰之組別，於初期並未提高酸鹼值，但於試驗期間仍維持pH6.0以上，且亦能快速吸附污染物，降低水相中之TCE濃度，顯示本基質具酸鹼緩衝之特性，而由分子生物結果顯示，添加兩種綠色基質皆能有效提升地下水體中脫氯相關菌群數量。證實綠色基質能提升物理、生物及化學三大面向之處理污染物的能力，具緩釋、pH及異味控制能力以提升含氯有機物之厭氧還原脫氯效率，且為對環境友善、綠色及永續之基質材料。

Trichloroethylene (TCE) is a common dense non-aqueous phase liquids (DNAPLs) pollutant in soil and groundwater. Enhanced anaerobic remediation is a better remediation treatment of TCE contaminated site. The first part of the study was a field model test using a long-lasting colloidal substrate. The injection of substrate can increase total organic carbon content to 1,126 mg/L (background value: 1.901 mg/L) at the initial stage, and quickly adsorb pollutants. After the 350 days, the degradation rate of the TCE reached 93% and maintained the pH value and the anaerobic reduction environment. Molecular biotechnology results shows that the significantly increased numbers of Enterobacter, methanogens and heterotrophic bacteria. It is confirmed that the base value can avoid water acidification, odor control and stimulate the growth of the existing dechlorination bacteria in the field and degrade TCE. The second part of the study is to use the unutilized resources of plants and the emulsifying substrate to synthesize the green substrate with buffering capacity and can slow-release carbon source. The results of microbial batch test showed that the addition of the plant ash group could provide alkalinity at the initial stage to neutralize the acidification problems of organic acids produced by fermentation, and the TCE degradation rate could reach 82.4% and 84.1%. The group of modified rice hull ash maintained pH above 6.0 during the test, and removed TCE concentration in the water phase quickly. Molecular biotechnology results show that the addition of two green matrices can increase the numbers of dechlorination-related bacteria. Green substrate is a environmentally friendly and sustainable material that has abilities of pH buffer, odor control and enhance reductive dechlorination efficiency.

目錄
學位論文審定書 i
公開授權書 ii
誌謝 iii
摘要 iv
ABSTRACT v
目錄 vi
圖目錄 ix
表目錄 xi
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 4
2.1含氯有機污染物 4
2.1.1含氯脂肪碳氫化合物污染概述 4
2.2三氯乙烯特性 9
2.2.1三氯乙烯物理化學特性及其對人體之風險危害 9
2.2.2三氯乙烯傳輸與環境風險危害 13
2.3土壤與地下水污染整治技術發展 15
2.3.1現地物理、化學及生物整治技術 15
2.3.2永續環境整治技術 17
2.4三氯乙烯生物降解機制 18
2.4.1好氧共代謝降解 18
2.4.2厭氧還原脫氯降解 20
2.5乳化型緩衝釋碳材 23
2.5.1長效型膠體基質 23
2.5.2草木灰 27
2.5.3改質稻殼灰 29
2.8分子生物技術於污染整治應用 32
第三章 材料與方法 34
3.1研究流程 34
3.2實驗材料與設備 36
3.2.1實驗材料 36
3.2.2實驗設備 38
3.3實驗基質製備 40
3.3.1奈米零價鐵 40
3.3.2植物油乳化基質 41
3.3.3長效型膠體基質 41
3.3.4綠色基質組 42
3.4模場試驗設計 43
3.4.1場址地質及水文介紹 43
3.4.2模場試驗方法 44
3.5批次試驗設計 46
3.5.1批次試驗規劃與方法 46
3.6實驗分析方法 48
3.6.1水質分析 48
3.6.2成分特性分析 52
3.6.3分子生物分析 54
第四章 結果與討論 60
4.1模場試驗 60
4.1.1現地地下水背景基本水質分析 62
4.1.2長效型膠體基質模場試驗基本水質分析 63
4.1.3長效型膠體基質模場試驗污染物降解成效 67
4.1.4長效型膠體基質模場試驗相關副產物變化 69
4.1.5分子生物技術分析成果 74
4.2綠色基質成分特性分析 77
4.2.1 ESEM-EDS 77
4.2.2 XRD 80
4.2.3 BET 81
4.3厭氧微生態批次試驗 82
4.3.1批次試驗基本水質分析 84
4.3.2批次試驗污染物濃度分析 89
4.3.3批次試驗水質及相關化學參數變化 93
4.3.4分子生物技術分析 98
4.4基質綜合效益評估 101
第五章 結論與建議 102
5.1結論 102
5.2建議 104
參考文獻 105



圖目錄
圖2-1 DNAPLs於地下污染分布 14
圖2-2 氧化共代謝簡易示意圖 19
圖2-3 共代謝過程的競爭抑制、還原能消耗再生及代謝產物毒性抑制示意圖 20
圖2-4 TCE氫解過程 21
圖2-5長效型膠體基質降解TCE機制圖 25
圖2-6 [SiO4 ]4-和[AlO4 ]5-晶體結構 29
圖3-1 研究架構流程圖 35
圖3-2 合成奈米零價鐵之反應器 38
圖3-3奈米零價鐵之製備過程照片 40
圖3-4 植物油乳化基質成品 41
圖3-5長效型膠體基質製備過程 42
圖3-6 (a)草木灰(b)改質稻殼灰 42
圖3-7現地模場整治井(RW為第一次注藥井)與監測井位置與地下水流向圖示 43
圖3-8 Pacbio 16S菌相分析流程圖 59
圖4-1 現地模場試驗之基本水質(a)pH及(b)ORP監測結果 65
圖4-2 現地模場試驗之基本水質(a)DO及(b)EC監測結果 66
圖4-3 現地地下水井TCE監測數據 68
圖4-4 現地地下水井(a)TOC及(b)甲烷監測數據 70
圖4-5 現地地下水井(a)cDCE及(b)1,1-DCE監測數據結果 71
圖4-6 硫化氫於不同酸鹼值條件下在水體中之型態與比例 72
圖4-7 現地試驗之硫化物監測濃度 73
圖4-8 模場Dhc基因表現量變化趨勢圖 74
圖4-9 藥井與其下游井於注藥前後之菌相豐富度變化圖 75
圖4-10 注藥井RW及其下游井之Heatmap圖 76
圖4-11 草木灰表面之E-SEM分析結果 78
圖4-12 草木灰表面之EDS分析結果 78
圖4-13 改質稻殼灰表面之E-SEM分析結果 79
圖4-14 改質稻殼灰表面之EDS分析結果 79
圖4-15 (a)草木灰及(b)改質稻殼灰之XRD晶相結構分析結果 80
圖4-16 批次試驗之基本水質(a)pH及(b)DO監測結果 87
圖4-17 批次試驗之基本水質(a)ORP及(b)EC監測結果 88
圖4-18 批次試驗之(a)TCE及(b)cDCE之監測結果 92
圖4-19 批次試驗之(a)TOC及(b)硫化物監測結果 95
圖4-20 批次試驗之(a)甲烷及(b)氫氣之監測結果 97
圖4-21 批次試驗Dhc基因表現量趨勢圖 100
 
表目錄

表 2-1 國內公告受CAHS之場址 6
表2-2 我國土壤及地下水中含CAHS污染管制標準 8
表2-3 含氯脂肪碳氫化合物性質與環境行為特點 9
表2-4 乙烯與氯化乙烯類化合物基本物化特性 11
表2-5 TCE之健康危害效應 12
表3-1井位相關參數 45
表3-2 批次實驗之組別 47
表3-3 菌屬及特徵基因於QPCR所使用之引子及探針序列 57
表3-4 REAL-TIME PCR所配置之反應混合液之比例 58
表3-5 NGS所使用之PRIMER 58
表4-1背景地下水採樣分析 62
表4-2 現地土壤分析 83
表4-3 現地地下水特性分析 83
表4-4 基質綜合評估 101

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