本研究之主要目的為瞭解奈米零價鐵做為氫氣提供來源，以加速含氯有機污染物於場址中自然衰減之可行性。本研究分為兩部份，第一部分的實驗中，以三氯乙烯(TCE, trichloroethylene)為目標污染物，利用生物批次實驗(microcosm)評估現地土壤與地下水在含有氫氣做為電子提供者下，與不同的氧化還原條件或是不同生物來源下，其降解程度之差別。第二部份之實驗則以批次實驗之方式，評估奈米零價鐵及奈米雙金屬產氫之可行性，並瞭解其產氫效率。
第一部分結果顯示，現地微生物於好氧及厭氧下皆具降解三氯乙烯之能力。此外，馴養後之好氧及厭氧污泥對三氯乙烯亦具良好之降解能力。以酚與糖蜜做為主要基質，可促進微生物好氧共代謝三氯乙烯。於厭氧狀態下，添加糖蜜及氫氣亦可促進現地微生物進行還原脫
氯作用去除三氯乙烯。添加奈米零價鐵之組別中，實驗組及控制組之三氯乙烯皆被完全降解。此結果顯示，奈米零價鐵之化學性還原脫氯作用為三氯乙烯被降解之優勢機制。因此，未來應提高三氯乙烯之濃度，或降低奈米零價鐵之添加劑量，以確實評估奈米零價鐵產生之氫
氣對三氯乙烯厭氧生物降解之影響。
第二部份結果顯示，零價鐵產氫效率大多高於50%，因此使用奈米零價鐵產氫為一有效率之產氫方式。而雙金屬奈米鐵產氫速率較一般奈米鐵佳，因此無論奈米零價鐵或雙金屬皆為優秀之釋氫物質。本研究結果顯示，奈米零價鐵為一優秀之釋氫物質。當含水層中注入適量奈米零價鐵時，其產生之氫氣可促進現地微生物之代謝，並幫助三氯乙烯之生物降解。使用奈米零價鐵之優點包括：(1)注入初期可迅速降低部份污染物濃度；(2)相較於貯存於鋼瓶之液態氫，奈米零價鐵提供氫氣之過程較為安全；及(3)可直接提供氫氣，氫氣產生過程無需進行微生物轉換機制。本研究成果顯示，以奈米零價鐵產氫促進現地微生物厭氧降解三氯乙烯應為一可行之方法。本研究之成果將可提供含氯有機物污染場址整治之參考。

The main objective of this study was to evaluate the feasibility of using nanoscale zero-valent iron (nZVI) as the source of hydrogen to enhance in situ anaerobic biodegradation of trichloroethylene (TCE). In the first part of this study, microcosms were constructed to evaluate the effects of different controlling factors [e.g., different redox conditions (aerobic and anaerobic conditions), different microorganisms (in situ microorganisms, activated sludge, and anaerobic sludge), and different sources of substrates and electron donors (phenol, cane molasses, hydrogen, and nZVI)] on TCE biodegradation. In the second part of this study, batch
experiments were conducted to evaluate the feasibility of hydrogen production by nZVI and bimetallic particles. Results from the microcosm study indicate that in-situ microorganisms were capable of degrading TCE under aerobic and anaerobic conditions. Results also show that TCE removal was more effective by activated sludge and anaerobic sludge. Aerobic biodegradation of TCE was
enhanced by the addition of phenol and cane molasses. Under anaerobic conditions, TCE removal could be improved when cane molasses and hydrogen were supplied. In addition, anaerobic TCE degradation was more effective with the presence of hydrogen. Results of microcosms conducted with the addition of nZVI reveal that TCE was degraded
completely in both live and autoclaved microcosms. This indicates that chemical reductive dechlorination seemed to dominate the removal of TCE in microcosms. Therefore, further studies with higher TCE concentrations or lower nZVI doses need to be conducted to determine the effects of the produced hydrogen on TCE biodegradation.
Results from the hydrogen production experiments indicate that efficiency of hydrogen production by nZVI ranged from 30% to 76%. Higher dose of nZVI addition resulted in higher amount of hydrogen
production. The total amounts of hydrogen production were correlated with the doses of nZVI. In addition, rates and efficiency of hydrogen production by bimetallic particles were better than those of nZVI. Results of the batch experiments reveal that nZVI and bimetallic particles had good efficiency on hydrogen production. This indicates that nZVI and bimetallic particles have high potential to be used as hydrogen producers.
In this study, a simple system consisted of only water and nZVI or bimetallic particles was applied to produce hydrogen. Although TCE in microcosms with nZVI addition was totally consumed by nZVI, results of
microcosms with hydrogen addition demonstrated that hydrogen was able to improve the efficiency of anaerobic TCE biodegradation. Thus, it may be feasible to use nZVI as the source of hydrogen to enhance in situ anaerobic biodegradation of TCE. The advantages of using nZVI as the source of hydrogen include: (1) rapid removal of significant contaminant
concentrations in the early stage of nZVI injection; (2) creation of a more reducing environment; (3) safer than liquid hydrogen, which is stored in steel containers; and (4) direct hydrogen supply without transfer of biological mechanisms compared to commercial hydrogen release compounds and other organic substrates. Results of this study suggest
that biological reductive dechlorination of TCE can be enhanced if proper doses of nZVI are supplied in situ. Knowledge and comprehension obtained in this study will be helpful in designing an enhanced in situ
anaerobic bioremediation system for a TCE-contaminated site.

謝誌............................................................................................................. I
摘要............................................................................................................II
Abstract .................................................................................................... IV
目錄.......................................................................................................... VI
圖目錄...................................................................................................... IX
表目錄........................................................................................................X
第一章 前言...............................................................................................1
1-1 研究緣起.......................................................................................1
1-1-1 氫氣促進生物降解.............................................................2
1-1-2 清淨能源............................................................................2
1-1-3 奈米零價鐵於環境整治上之應用....................................3
1-2 研究目的......................................................................................4
第二章 文獻回顧......................................................................................5
2-1 地下水污染..................................................................................5
2-2 地下水污染中三氯乙烯之來源...................................................6
2-2-1 三氯乙烯之化學性質......................................................11
2-3 三氯乙烯之生物處理技術........................................................15
2-3-1 影響生物降解之因子......................................................15
2-3-2 加強式生物處理法..........................................................19
2-3-3 三氯乙烯好氧與厭氧下之代謝......................................19
2-3-4 三氯乙烯之生物共代謝作用..........................................20
2-3-5 現地整治牆之應用..........................................................20
2-4 以零價鐵處理三氯乙烯污染之地下水....................................24
2-4-1 奈米級零價鐵之特性......................................................25
2-4-2 氫氣對於微生物代謝之影響..........................................25
2-4-3 以氫氣作為清淨能源之可行性......................................26
第三章 實驗設備與方法......................................................................28
3-1 實驗材料....................................................................................28
3-1-1 實驗用水與微生物來源..................................................28
3-1-2 添加碳源..........................................................................28
3-1-3 緩衝劑..............................................................................28
3-1-4 三氯乙烯..........................................................................29
3-1-5 奈米零價鐵......................................................................29
3-2 實驗設備....................................................................................29
3-2-1 合成奈米零價鐵反應器..................................................29
3-2-2 氣相層析儀/電子捕捉偵測器.........................................31
3-2-3 壓力計..............................................................................32
3-3 實驗方法與步驟........................................................................33
3-3-1 奈米零價鐵與雙金屬零價鐵製備..................................33
3-3-2 三氯乙烯之好氧降解......................................................34
3-3-3 三氯乙烯之厭氧降解......................................................37
3-3-4 零價鐵之產氫效率實驗..................................................41
3-3-5 實驗研究架構..................................................................41
第四章 結果與討論..............................................................................44
4-1 微生物好氧環境降解三氯乙烯................................................44
4-1-1 好氧酚共代謝組結果......................................................44
4-1-2 好氧糖蜜共代謝組結果..................................................45
4-1-3 好氧生物降解組結果......................................................45
4-1-4 好氧污泥生物降解組結果..............................................45
4-1-5 好氧污泥糖蜜生物共代謝組結果..................................46
4-2 微生物厭氧環境降解三氯乙烯................................................49
4-2-1 厭氧糖蜜共代謝組結果..................................................49
4-2-2 厭氧添加氫氣生物降解組結果......................................49
4-2-3 奈米零價鐵與生物降解組結果......................................50
4-2-4 厭氧污泥生物降解組結果..............................................50
4-2-5 厭氧污泥糖蜜生物共代謝組結果..................................51
4-2-6 土壤厭氧生物降解組結果..............................................51
4-3 產氫實驗結果............................................................................57
4-3-1 奈米零價鐵產氫結果......................................................57
4-3-2 雙金屬零價鐵產氫結果..................................................58
4-3-3 實驗結果討論..................................................................60
第五章 結論與建議..............................................................................61
5-1 結論............................................................................................61
5-2 建議............................................................................................63
參考文獻...................................................................................................64
附錄...........................................................................................................74

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