本研究利用化學還原法以試藥級試劑製備之奈米級零價鐵(NZVI)，經場發射型掃描式電子顯微鏡分析後粒徑介於50∼80 nm間，比表面積測值66.34 m2/g；採工業級試劑合成之NZVI粒徑分布範圍略廣(30∼80 nm)，比表面積測值61.5 m2/g，由氮氣吸/脫附曲線結果顯示兩種NZVI之顆粒表面皆呈介孔性結構，顯示其基本特性與試藥級試劑合成之NZVI所得差異不大，適宜作為實際整治之應用。
製備穩定性高之奈米級零價鐵懸浮液(NZVIS)試驗過程中，結果顯示於製備過程中添加0.5 vol %陰離子型親水性界面活性劑(分散劑A)合成之NZVIS具有較佳之穩定性，顆粒粒徑較小且分布均勻。
以NZVI為還原劑，三氯乙烯(TCE)降解反應過程中產生之中間產物以cis-1,2-DCE為主，亦有少量的trans-1,2-DCE產生，但兩物種濃度皆隨時間增長而遞減，並不會持續累積在反應系統中。此外，碳氫化合物之副產物以甲烷為主，且反應系統中若有氫氣存在者，有微量之乙烷、乙烯產生，推測係H2(g)參與反應，促進氫化反應進行。
使用奈米級鈀/鐵雙金屬降解TCE時，在含有氫氣之條件下，氫氣濃度越高者，TCE降解速率越快，然而含氯中間副產物(DCEs)濃度也越高，顯示氫解作用為優勢反應，反應3分鐘後，TCE去除效率高達99 %；就碳氫化合物而言，副產物以乙烷為主，證實鈀催化劑存在會促使TCE直接降解成乙烷。
添加NZVIS於土壤中(鐵相對於土壤之重量為2.5×10-3)經培養後顯示，含有少量NZVIS者，其總菌落數較未添加者高，即NZVIS對土壤中總菌落數而言，並不會造成抑制生長或削減活性的情形發生。
改質之NZVIS在多孔介質中的垂直傳輸結果得知，本研究於製備過程中所使用的分散劑A能使NZVIS均勻流佈在石英砂管柱中，黏附係數值為0.11，此一數值較未使用分散劑改值前之黏附係數值0.56為低；而在土壤(壤質砂土)管柱中傳輸之黏附係數值為0.0061，顯示本研究自行製備之NZVIS於多孔介質中能有良好的傳輸特性。
施加電場於水平土壤管柱之作用下， NZVIS於傳輸過程所求得之黏附係數值為0.00034，鐵含量亦減少了10 %，顯示施加電場不僅能驅動懸浮液在水平管柱中的移動，亦可提升NZVI於多孔介質中的傳輸特性。

In this research, nanoscale zero-valent iron (NZVI) was synthesized using the chemical reduction method. Experimental results have revealed that nanoiron synthesized by the reagent-grade chemicals had a size range of 50-80 nm, as determined by FE SEM. BET specific surface area of thus synthesized nanoparticles was 66.34 m2/g. NZVI prepared by the industrial-grade chemicals had a broader particle size distribution (30-80 nm) and its BET specific surface area was 61.50 m2/g. Results of XRD showed that both types of NZVI were composed of iron with a poor crystallinity. Additional test results further showed that both types of NZVI had similar characteristics.
NZVI prepared by the chemical reduction method tends to aggregate resulting in a significant loss in reactivity. To overcome this disadvantage, four water-soluble dispersants were used in different stages of the NZVI preparation process. Of these, Dispersant A (an anionic surfactant) has shown its superior stabilizing capability to others. An addition of 0.5 vol % Dispersant A during the nanoiron preparation process would result in a good stability of NZVI slurry (NZVIS).
Degradation of trichloroethylene (TCE) by NZVIS under different atmospheres was carried out in batch experiments. Experimental results have shown that the TCE dechlorination rate increased markedly when the reaction proceeded under hydrogen gas atmosphere as compared with that of air. Methane was the primary end product with a trace amount of ethane and ethylene when the reaction was conducted under the atmosphere of H2. It was suggested that an addition of H2 to the reaction system could promote the hydrogenolysis reaction for better degradation. On the other hand, ethane was the main product when the reaction system consisted of nanoscale palladized iron and H2 atmosphere. It demonstrated that Pd-catalyzed TCE dechlorination has resulted in a direct conversion of TCE to ethane in the study. The greatest dechlorination rate was obtained when 2 g/L nanoscale palladized iron and 50 mL H2 was employed in the reaction system. Under the circumstances, the TCE (10 mg/L) removal efficiency was up to 99 % in 3 minutes. Experimental results have demonstrated that the reaction system with both nanoscale palladized iron and H2 atmosphere would promote TCE degradation rate.
The culture of microorganism in soil showed minor changes to microbial community structures between the pre- and post-injection conditions. The number of microorganism colony was found to be increased after adding 1 mL NZVIS to 1 g soil. Experimental results revealed that NZVIS would not cause the inhibition or reduction of microorganism activity.
Surface modification of NZVI slurry by Dispersant A could enhance its transport in saturated porous media. Sticking coefficients were determined to be 0.56 and 0.11, respectively, for bare and Dispersant A-modified NZVIS transporting in quartz sand columns. The sticking coefficient for modified NZVIS transport in soil (loamy sand) column was determined to be 0.0061. Apparently, NZVIS modified by Dispersant A would enhance the transport of NZVI in saturated porous media.
The results of combining electrokinetic technology and NZVIS injection tests in horizontal soil column illustrated that the sticking coefficient was 0.00034 and the total content of iron reduced 10 wt. %. Experimental results revealed that the transport distance of NZVIS in saturated horizontal soil column would be greatly increased under electronkinetic conditions.

聲明切結書 I
謝誌 II
摘要 III
ABSTRACT IV
目錄 VI
表目錄 IX
圖目錄 X
照片目錄 XII
第一章 前言 1
1-1 研究緣起 1
1-2 研究目的 4
1-3 研究項目與架構 5
第二章 文獻回顧 7
2-1 含氯有機化合物 7
2-1-1 含氯有機化合物之特性與危害 7
2-1-2 含氯有機化合物之污染與管制 10
2-1-3 三氯乙烯(TCE) 13
2-1-4 受含氯有機化合物污染之整治技術 15
2-2 零價金屬處理技術與發展 18
2-2-1 零價鐵之應用原理 18
2-2-2 零價鐵處理之反應機制 20
2-3 奈米鐵之技術與發展 24
2-3-1 奈米技術 24
2-3-2 奈米金屬材料製備相關技術 27
2-3-3 奈米金屬材料分散性能探討 30
2-4 雙金屬之技術原理與發展 34
2-4-1 雙金屬的合成 34
2-4-2 雙金屬對污染物之降解原理 36
2-5 含氯有機化合物之降解機制 40
2-6 傳輸特性探討 44
第三章 研究方法 50
3-1 研究內容 50
3-2 研究材料 51
3-2-1 化學藥劑 51
3-2-2 其他材料 54
3-3 研究設備 55
3-4 研究方法 57
3-4-1奈米級零價鐵與鈀/鐵雙金屬之合成 57
3-4-2 奈米鐵及鈀/鐵雙金屬基本性質分析 59
3-4-3奈米鐵懸浮液之穩定性探討 62
3-4-4 檢量線之建立 66
3-4-5 TCE降解批次實驗 73
3-4-6 土壤中總生菌數檢測 76
3-4-7 NZVIS於土壤中之傳輸 78
第四章 結果與討論 84
4-1 奈米級零價鐵與鈀/鐵雙金屬基本特性分析 84
4-1-1 X-光繞射分析物種成分 84
4-1-2 場發射型掃描式電子顯微鏡(FE SEM)觀察顆粒型態 86
4-1-3 BET比表面積分析 88
4-1-4 掃描式電子顯微鏡-X-光能譜分析儀(SEM-EDS)與能量分佈面掃描分析(EDS-Mapping) 90
4-2 奈米鐵懸浮液之穩定性探討 96
4-2-1沉降試驗 97
4-2-2動態光散射(Dynamic Light Scattering, DLS) 99
4-3 不同環境氣氛下奈米級零價鐵及鈀/鐵雙金屬懸浮液降解水溶液中之三氯乙烯 102
4-3-1未添加任何還原劑之背景試驗 104
4-3-2試藥級藥品合成之懸浮液於不同環境氣氛下降解水溶液中之三氯乙烯 106
4-3-3工業級藥品合成之懸浮液於不同環境氣氛下降解水溶液中之三氯乙烯 117
4-4 三氯乙烯降解反應路徑與機制探討 120
4-4-1 奈米級零價鐵還原處理三氯乙烯之反應機制探討 120
4-4-2 奈米級鈀/鐵雙金屬還原處理三氯乙烯之反應機制探討 123
4-5 奈米級鐵懸浮液對土壤環境中總菌落數之影響 126
4-6 奈米級零價鐵懸浮液於土體中之傳輸特性 132
4-6-1 奈米級零價鐵懸浮液於不同多孔介質中之垂直傳輸情形 132
4-6-2 黏附係數(Sticking Coefficient,α)計算 136
4-6-3 在電場作用下NZVIS於土壤管柱中之水平傳輸情形 137
第五章 結論與建議 142
5-1 結論 142
5-2 建議 144
參考文獻 145
附錄 161
碩士在學期間發表之學術論文 162

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