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研究生:蘇致綱
研究生(外文):Chih-Gang Su
論文名稱:奈米零價鐵複合活性碳處理三氯乙烯污染物之評估
論文名稱(外文):Evaluation of activated carbon supported nanoscale zero valent iron for treating trichloroethylene
指導教授:梁振儒梁振儒引用關係
學位類別:碩士
校院名稱:國立中興大學
系所名稱:環境工程學系所
學門:工程學門
學類:環境工程學類
論文種類:學術論文
論文出版年:2009
畢業學年度:97
語文別:中文
論文頁數:136
中文關鍵詞:地下水污染氯化有機溶劑零價鐵吸附透水性反應牆
外文關鍵詞:Groundwater contaminationChlorinated solventZero valent ironAdsorptionPermeable reactive barrier
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三氯乙烯(TCE)為土壤及地下水中常見之有機氯化溶劑污染物,屬比水重非水相液體,若意外洩漏至地表下,將成為土壤與地下水長期之污染源。透水性反應牆(PRB)為一被動式之土壤及地下水污染整治方法,零價鐵(ZVI)與活性碳(AC)為PRB廣泛採用之填充材質,其中ZVI可藉由表面與污染物接觸,對TCE進行還原脫氯反應,以達到降解污染物之目的,且其反應性與表面積呈正相關。此外AC則藉由其多孔隙與具多種表面官能基之特性,可經物理及化學性吸附,將污染物移除。本研究嘗試將奈米級零價鐵(nZVI)披覆至活性碳上,並對於此複合材料其結合吸附及還原反應用以處理TCE污染之效能進行評估。
實驗結果顯示,使用硼氫化鈉還原法將nZVI披覆至AC上為一可行之製備程序,且經掃描式電子顯微鏡分析,得知不同鍛燒溫度下所製備得之複合材料上nZVI之粒徑約為50-100nm;此外分散劑聚乙二醇於製備程序中之使用,對於nZVI粒徑大小並無明顯影響,但可得較佳之nZVI於AC上之分散性。nZVI/AC複合材料降解TCE所生成之降解產物氯離子與僅nZVI存在下所得之結果相較,可知複合材料具較佳之Cl-生成程度;反應過後之複合材料,可藉由熱碳還原法予以再生利用,提供此複合材料回收再利用之方法。
Chlorinated solvents such as trichloroethylene (TCE) are among the most common soil and groundwater contaminants. If TCE, as a dense non-aqueous phase liquid, is accidently released in the subsurface, its presence would become a continuous source of contamination. Permeable reactive barrier (PRB) is a passive technology for in situ clean-up of groundwater contamination. Among reactive materials filled within PRB, zero valent iron (ZVI) and activated carbon (AC) are widely used reactive materials. ZVI undergoes reductive dechlorination of TCE when containments are in contact with ZVI surface. Therefore, specific surface area of ZVI is highly correlated with high reactivity. In addition, AC with high surface area and multiple surface functional groups is a good adsorbent for removing contaminants. In this study, a process of coating nano zero valent iron (nZVI) onto AC, namely nZVI/AC, was developed. Then evaluation of the synthesized nZVI/AC composites for remediating TCE contamination was conducted.
The results present a successful approach of combining impregnation and borohydride reduction to synthesize nZVI/AC composites. SEM analysis demonstrates that the size of nZVI on AC synthesized under different calcined temperatures is about 50-100 nm. Furthermore, the addition of polyethylene glycol dispersant for preparation of nZVI/AV reveals no effect on nZVI particle size. However, a well dispersion of nZVI on AC is achieved. When comparing nZVI/AC to nZVI on degradations of TCE, nZVI/AC reveals higher percentage of dechlorination than using nZVI only. The used nZVI/AC composites can then be regenerated by carbothermal reduction process which can be an effective method to regenerate the synthesized nZVI/AC composites.
目錄
中文摘要 I
Abstract II
目錄 II
表目錄 VI
圖目錄 VIII
第一章 緒論 1
1-1 研究緣起 1
1-2 研究目的 3
第二章 文獻回顧 4
2-1 三氯乙烯污染 4
2-1-1 三氯乙烯之物化特性與危害性 4
2-1-2 三氯乙烯污染狀況 6
2-2 土壤及地下水整治方法 11
2-2-1 物理化學復育處理 11
2-2-2 生物復育處理 15
2-3 活性碳 17
2-3-1 活性碳吸附行為 17
2-3-2 活性碳等溫吸附模式 19
2-4 零價鐵 22
2-4-1 零價鐵特性與反應機制 24
2-4-2 奈米級零價鐵 37
2-4-3 零價鐵複合材料 41
第三章 實驗材料與方法 43
3-1 實驗材料與設備 43
3-2 實驗流程 45
3-2-1 nZVI/AC複合材料製備 46
3-2-2 nZVI/AC降解三氯乙烯 49
3-2-3 nZVI/AC吸附三氯乙烯 51
3-2-4 nZVI/AC劑量對降解三氯乙烯影響 52
3-2-5 TCE降解副產物分析 52
3-2-6 nZVI/AC複合材料之再生 54
3-3 實驗分析方法 56
第四章 結果與討論 64
4-1 nZVI/AC複合材料特性分析 64
4-2 nZVI/AC複合材料降解三氯乙烯效率評估 85
4-2-1 nZVI/AC降解三氯乙烯 85
4-2-2 nZVI/AC反應後之特性分析 90
4-3 nZVI/AC複合材料吸附三氯乙烯 100
4-3-1 nZVI/AC吸附動力 100
4-3-2 nZVI/AC等溫吸附 101
4-4 nZVI/AC複合材料劑量對降解三氯乙烯之影響 103
4-5 nZVI/AC複合材料降解三氯乙烯副產物分析 108
4-6 nZVI/AC複合材料再生 113
4-6-1 再生之複合材料特性分析 113
4-6-2 再生之複合材料降解三氯乙烯 120
第五章 結論與建議 122
5-1 結論 122
5-2 建議 124
第六章 參考文獻 125

表目錄
表2-1 三氯乙烯物化特性 5
表2-2 三氯乙烯對人體危害性 6
表2-3 環保署公告受三氯乙烯污染之場址 10
表2-4 污染物與適用之填充材質 15
表2-5 活性碳孔徑大小、體積與比表面積 18
表2-6 物理性與化學性吸附差異 19
表2-7 ZVI降解TCE常見之副產物 33
表2-8 ZVI降解TCE之反應速率常數 38
表3-1 nZVI/AC 複合材料製備實驗參數 47
表3-2 nZVI/AC降解TCE實驗參數 50
表3-3 nZVI/AC吸附實驗參數 52
表3-4 nZVI/AC降解TCE實驗參數 53
表3-5 nZVI/AC再生實驗參數 55
表3-6 再生之nZVI/AC複合材料降解TCE實驗參數 55
表4-1 nZVI/AC複合材料BET與孔隙體積變化 80
表4-2 利用PEG製備ZVI或氧化鐵FTIR分析之官能基及吸收波數 83
表4-3 nZVI/AC複合材料之反應速率常數(kobs, TCE) 86
表4-4 nZVI/AC複合材料反應前後含鐵量 98
表4-5 Freundlich與Langmuir吸附模式參數 102
表4-6 不同劑量之nZACP700與TCE反應條件下,Cl-生成反應速率常數 107

圖目錄
圖2-1 各類應徵收化學物質繳交整治費比例圖 8
圖2-2 地下水污染場址各類污染項目比例 8
圖2-3 DNAPL於地表下的傳輸途徑 9
圖2-4 透水性反應牆示意圖 14
圖2-5 透水性反應牆型式 14
圖2-6 零價鐵結合生物系統降解硝酸鹽 16
圖2-7 活性碳孔隙結構圖 17
圖2-8 活性碳上常見之官能基 18
圖2-9 零價鐵實場應用操作方式 23
圖2-10 污染物與零價鐵接觸過程示意圖 25
圖2-11 零價鐵反應機制 26
圖2-12 零價鐵表面電子轉移途徑 27
圖2-13 ZVI降解TCE反應途徑 31
圖2-14 零價鐵核殼結構 37
圖2-15 PEG結構式 40
圖2-16 GAC/ZVI/Pd複合材料處理二氯聯苯示意圖 42
圖3-1 實驗設計流程圖 45
圖3-2 nZVI/AC複合材料製備反應器配置圖 48
圖3-3 nZVI/AC降解TCE反應器配置圖 51
圖3-4 高溫管狀爐鍛燒裝置圖 54
圖3-5 TCE之GC-FID層析圖譜範例 57
圖3-6 TCE檢量線範例 57
圖3-7 Cl-之IC層析圖譜範例 58
圖3-8 氯離子檢量線範例 58
圖4-1 活性碳之SEM/SEI影像 64
圖4-2 活性碳之EDS圖譜 65
圖4-3 nZVI之SEM/SEI影像 (a)50000倍及(b)100000倍 66
圖4-4 nZVI/AC複合材料之SEM/BEI影像250倍 67
圖4-5 nZVI/AC複合材料之SEM/BEI影像1500倍 68
圖4-6 nZVI/AC複合材料之SEM/SEI影像50000倍 70
圖4-7 nZVI/AC複合材料之SEM/BEI影像 70
圖4-8 nZAC105之EDS圖譜 71
圖4-9 nZAC700之EDS圖譜 72
圖4-10 nZACP105之EDS圖譜 73
圖4-11 nZACP700之EDS圖譜 74
圖4-12 nZVI之TEM影像 (a)100000倍及(b)400000倍 75
圖4-13 nZVI/AC複合材料之TEM影像25000倍 76
圖4-14 nZVI/AC複合材料之TEM影像100000倍 77
圖4-15 nZVI/AC複合材料之氮氣吸脫附曲線 78
圖4-16 等溫吸附類型分類 79
圖4-17 nZVI/AC複合材料孔隙直徑與體積之變化 80
圖4-18 nZVI/AC複合材料之XRD分析圖譜 81
圖4-19 nZVI/AC複合材料之FTIR官能基分析圖譜 84
圖4-20 nZVI/AC複合材料降解TCE反應過程中,TCE隨時間之變化 86
圖4-21 nZVI/AC複合材料降解TCE反應過程中,Cl-隨時間之變化,內插圖為Cl-(C/C0)與時間之變化關係 87
圖4-22 TCE吸附及脫氯程度之質量平衡 88
圖4-23 nZVI/AC複合材料降解TCE反應過程中,ORP隨時間之變化 89
圖4-24 nZVI/AC複合材料降解TCE反應過程中,pH隨時間之變化 89
圖4-25 nZVI/AC複合材料之SEM/BEI影像250倍 91
圖4-26 nZVI/AC複合材料之SEM/SEI影像 92
圖4-27 RnZAC105之EDS圖譜 93
圖4-28 RnZAC700之EDS圖譜 94
圖4-29 RnZACP105之EDS圖譜 95
圖4-30 RnZACP700之EDS圖譜 96
圖4-31 nZVI/AC複合材料反應後之XRD分析圖譜 97
圖4-32 nZVI/AC複合材料反應前後含鐵量質量平衡關係圖 99
圖4-33 TCE吸附動力曲線 100
圖4-34 TCE 之Freundlich等溫吸附曲線 101
圖4-35 TCE之 Langmuir等溫吸附曲線 102
圖4-36 不同劑量之nZACP700與TCE反應條件下,水溶相TCE隨時間之變化,內插圖為局部數據放大圖 103
圖4-37 不同劑量之nZACP700與TCE反應條件下,pH隨時間變化 104
圖4-38 不同劑量之nZACP700與TCE反應條件下,Cl-生成隨時間之變化 106
圖4-39 不同劑量之nZACP700與TCE反應條件下,TCE吸附及Cl-生成之脫氯程度質量平衡 107
圖4-40 TCE及部分降解副產物標準品定性GC/FID分析圖譜 109
圖4-41 nZACP700降解TCE,於不同反應時間條件下氣相GC/FID分析圖譜 110
圖4-42 nZACP700降解TCE,於不同反應時間條件下液相經P&T前處理之GC/FID分析圖譜 111
圖4-43 nZACP700降解TCE,於不同反應時間條件下固相經Methanol萃取之GC/FID分析圖譜 112
圖4-44 再生之複合材料SEM/BEI影像250倍 113
圖4-45 再生之複合材料SEM/BEI影像1500倍 114
圖4-46 再生之複合材料SEM影像 115
圖4-47 RnZAC700-RE500之EDS圖譜 116
圖4-48 RnZAC700-RE700之EDS圖譜 117
圖4-49 RnZAC700-RE1000之EDS圖譜 118
圖4-50 高溫再生之複合材料XRD分析圖譜 119
圖4-51 再生之複合材料與TCE反應過程中,TCE隨時間之變化,內插圖為ORP隨時間之變化 120
圖4-52 再生之複合材料反應過程中,pH隨時間變化 121
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