臺灣博碩士論文加值系統

本研究利用奈米級Fe3O4懸浮液活化過硫酸鹽整治受三氯乙烯(TCE)及1,2-二氯乙烷(1,2-DCA)污染之水溶液及飽和土壤，首先，本研究以化學共沉澱法自行合成奈米級Fe3O4，並在晶型鑑定及尺寸分析確定其為奈米級Fe3O4後，利用環境友善性的可溶性澱粉進行分散性試驗，確保其穩定性，結果顯示，於合成過程中添加3 wt%之可溶性澱粉可有效將奈米級Fe3O4分散並且達到一個月以上的懸浮效果。
接著，利用製備完成的奈米級Fe3O4活化過硫酸鹽處理水溶液(DI水、模擬地下水及實際地下水)中的TCE及1,2-DCA，其整治效率皆可達到95 %以上；本研究並偵測利用過硫酸鹽氧化破壞TCE及1,2-DCA所產生的中間產物，其主要的第一階中間產物為cis-1,2-DCA及trans-1,2-DCE，而後，再氧化破壞成第二階中間產物(VC)， VC甚至再被氧化破壞成更安全且穩定的物質(乙烷、乙烯及甲烷)。
而後，利用奈米級Fe3O4懸浮液及過硫酸鹽注入結合電動力法處理飽和土壤中的TCE及1,2-DCA。由結果顯示，添加過硫酸鹽可有效降低電極極化現象，進而增加每日電滲透流流量及電流密度；於陰極槽注入過硫酸鹽並產生的硫酸根自由基(SO4-‧)，會隨電動力法之離子遷移機制進入土壤管柱並移除標的污染物，相較於陽極槽注入，陰極槽注入有較佳的整治效果；分別於電動力整治系統之陰、陽極槽注入過硫酸鹽及奈米級Fe3O4懸浮液處理受污染的土壤，其移除效率皆可達96 %以上。
為了探討本電動力整治系統是否可有效應用於實際污染場址，本研究特別配製高濃度污染土並予陳化一週，並結合上述電動力整治系統所選擇之最佳條件進行經陳化作用後之試驗。試驗結果發現，標的污染物TCE及1,2-DCA皆可符合土壤污染管制標準，並且在電動力整治系統進行30日後，其中間產物(cis-1,2-DCA、trans-1,2-DCE及VC)皆可有效移除，並低於土壤污染管制標準。
此外，本研究為了證實本電動力整治系統之經濟可行性，因此，將各試驗進行操作費用(藥品費用 + 電費)評估，其結果顯示，操作費用約為8000-17000 元/m3，具有經濟可行性。

The purpose of this work was to investigate the use of nanoscale Fe3O4 as a catalytst for destruction of trichloroethylene (TCE) and 1,2-dichloroethane (1,2-DCA) by persulfate in spiked water and soil. First, nanoscale Fe3O4 was prepared by chemical coprecipitation. X-ray powder diffraction (XRD) was used to confirm the crystal structure; And size identification was performed using the scanning electron microscopy (SEM).
The effectiveness of using 3 wt% soluble starch (SS) to stabilize nanoscale Fe3O4 was also studied. It was found that SS could effectively disperse the nanoparticles for more than one month. Therefore, SS was chosen to prepare the nanoscale Fe3O4 slurry.
The efficiency of nanoscale Fe3O4 as an activator for persulfate remediation of TCE and 1,2-DCA in aqueous solutions (DI water, simulated groundwater, and actual groundwater) was then investigated. The results showed that all test removal efficiency of TCE and 1,2-DCA was more than 95%. Use of the persulfate for destruction of TCE and 1,2-DCA produced some by-products. The primary reaction products were cis-1,2-Dichloroethylene (cis-1,2-DCE) and trans-1,2-Dichloroethylene (trans-1,2-DCE)； The secondary daughter prodnct was vinyl chloride (VC). The VC produced is gradually degraded to safer substances (ethene, ethane, and methane).
The nanoscale Fe3O4 slurry and the persulfate injection coupled with the electrokinetic (EK) process was tested for remediation of TCE and 1,2-DCA in saturated soil. The results showed that injection of persulfate into the EK reservoir could decrease the electrode polarization, and increase the electroosmotic flow and current density. When persulfate was injected into the cathode reservoir, the derived sulfate radicals would transfer into the soil compartment by ion migration.
The injection of persulfate into the cathode reservoir was more efficient than injection of persulfate into the anode reservoir. The removal efficiency for TCE and 1,2-DCA was more than 96% in all tests.
The remediation system was assessed for potential application in-situ. Soil was spiked with high TCE and 1,2-DCA and aged for a week. The injection of persulfate and nanoscale Fe3O4 slurry coupled with the EK process was tested for remediation of the aged contaminated soil. The results showed that the target contaminants (TCE and 1,2-DCA) met the Taiwan’s EPA’s control standard. After 30 d of remediation, the by-products (cis-1,2-DCE, trans-1,2-DCE, and VC) had also been removed to below the action limit.
A cost analysis was performed in order to demonstrate the economic feasibility of the remediation method in this study. Operating costs (chemicals + electricity bill) of all tests were assessed. The results showed that the costs were 8000-17000 NT$/m3, which is economically reasonable.

聲明切結書 .............................................................................................i
謝誌 ........................................................................................................ ii
摘要 ....................................................................................................... iii
ABSTRACT ........................................................................................... v
目錄 ...................................................................................................... vii
表目錄 ................................................................................................... ix
圖目錄 ................................................................................................... xi
照片目錄............................................................................................... xv
第一章 前言 .......................................................................................... 1
1.1 研究緣起 ...................................................................................... 1
1.2 研究目的 ...................................................................................... 3
1.3 研究架構 ...................................................................................... 4
第二章 文獻回顧 .................................................................................. 6
2.1 含氯有機化合物 .......................................................................... 6
2.1.1 含氯碳氫有機化合物之特性及危害 ..................................... 6
2.1.2 含氯碳氫有機化合物之污染及管制 ..................................... 7
2.1.3 三氯乙烯(TCE) ..................................................................... 10
2.1.4 1,2-二氯乙烷(1,2-DCA) ..................................................... 11
2.1.5 整治受含氯有機化合物污染之技術應用 ........................... 14
2.2 現地整治技術之原理及發展 .................................................... 15
2.3 現地氧化技術 ............................................................................ 17
2.3.1 高級氧化技術(AOPs)之發展與應用 ................................... 17
2.3.2 過硫酸鹽之反應機制 ........................................................... 22
2.3.3 過硫酸鹽之應用 ................................................................... 25
2.4 電動力法 .................................................................................... 26
2.4.1 電動力整治技術原理 ........................................................... 27
2.4.2 電動力法傳輸與反應機制 ................................................... 28
2.4.3 電動力整治技術之發展 ....................................................... 33
2.5 奈米技術與發展 ........................................................................ 34
2.5.1 四氧化三鐵 ........................................................................... 35
2.5.2 奈米級四氧化三鐵的發展及應用 ....................................... 36
2.5.3 奈米級四氧化三鐵之合成 ................................................... 37
2.6 含氯有機化合物之降解機制 .................................................... 38
第三章 實驗材料與方法 .................................................................... 40
3.1 實驗材料 .................................................................................... 40
3.2 實驗設備 .................................................................................... 43
3.2.1 儀器設備 ............................................................................... 43
3.2.2 電動力管柱之處理系統 ....................................................... 46
3.3 實驗方法 .................................................................................... 48
3.3.1 過硫酸鹽溶液之製備 ........................................................... 48
3.3.2 奈米級Fe3O4之製備 ............................................................ 49
3.3.2.1 粒徑大小與型態及其元素分析 ................................... 50
3.3.2.2 晶型鑑定 ....................................................................... 50
3.3.2.3 利用可溶性澱粉製備奈米材料懸浮液 ....................... 51
3.3.3 模擬地下水之製備 ............................................................... 52
3.3.4 利用奈米級Fe3O4活化過硫酸鹽氧化三氯乙烯及1,2- 二氯乙烷水溶液詴樣之批次詴驗 ........................................ 54
3.3.5 過硫酸鹽及奈米級Fe3O4懸浮液注入結合電動力法 整治模擬受三氯乙烯及1,2-二氯乙烷之飽和土壤之 詴驗 .............................................................................................. 57
3.3.5.1 土壤對三氯乙烯及1,2-二氯乙烷之吸附性詴驗 ....... 58
3.3.5.2人工污染土壤製備與管柱裝填 .................................... 60
3.3.5.3 實驗進行反應過程分析項目 ....................................... 61
3.3.5.4 TCE及1,2-DCA及其副產物檢量線建立 .................. 62
3.3.5.5 實驗進行前後之土壤分析項目 ................................... 63
3.3.6 奈米材料與過硫酸鹽分別注入結合電動力法整治 模擬受三氯乙烯及1,2-二氯乙烷之陳化飽和土壤 之詴驗 .......................................................................................... 70
第四章 結果與討論 ............................................................................ 71
4.1 奈米級Fe3O4之基本特性分析 ................................................. 71
4.1.1. 場發射型掃描式電子顯微鏡(TF SEM) ............................. 71
4.1.2. 環境掃描式電子顯微鏡-能量分散光譜儀分析 ................. 73
4.1.3. X-光繞射儀分析(XRD) ........................................................ 74
4.2 利用可溶性澱粉製備奈米級Fe3O4懸浮液之懸浮性探討..... 75
4.3 土壤之基本特性分析 ................................................................ 81
4.4 利用奈米級Fe3O4活化過硫酸鹽氧化受三氯乙烯及 1,2二氯乙烷污染之模擬水溶液詴樣之批次成效探討 ........... 83
4.4.1利用奈米級Fe3O4活化過硫酸鹽氧化受三氯乙烯及 1,2-二氯乙烷污染於去離子水之批次成效探討 ................... 84
4.4.2利用奈米級Fe3O4活化過硫酸鹽氧化受三氯乙烯及
1,2-二氯乙烷污染於不同地下水之處理成效探討 ............... 87
4.4.3利用奈米級Fe3O4活化過硫酸鹽處理受TCE及 1,2-DCA污染的水樣所產生的中間產物探討 ...................... 93
4.5 土壤對三氯乙烯及1,2-二氯乙烷之吸附性詴驗 .................. 104
4.6 過硫酸鹽注入結合電動力法模擬現地整治飽和土壤中 之三氯乙烯及1,2-二氯乙烷詴驗 ............................................ 107
4.7 過硫酸鹽及奈米級Fe3O4懸浮液注入結合電動力法 模擬現地整治經陳化作用後的飽和土壤中之TCE及 1,2-DCA之詴驗 ........................................................................ 127
4.7.1過硫酸鹽及奈米級Fe3O4懸浮液注入結合電動力法 模擬現地整治經14日陳化作用後的飽和土壤中之 TCE及1,2-DCA之成效探討 .............................................. 129
4.7.2 過硫酸鹽及奈米級Fe3O4懸浮液注入結合電動力法 模擬現地長期整治30日經陳化作用後的飽和 土壤中之TCE及1,2-DCA之成效探討 ................................. 140
4.8 操作費用之評估與比較 .......................................................... 149
第五章 結論與建議 .......................................................................... 152
5.1 結論 .......................................................................................... 152
5.2 建議 .......................................................................................... 155
參考文獻............................................................................................. 156
附錄 ..................................................................................................... 172
碩士在學期間發表之學術論文 ........................................................ 175

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