本研究是以奈米級複合金屬進行污染物的降解去除，以土壤地下水中常見之污染物三氯乙烯及六價鉻作為目標污染物進行實驗，奈米金屬於污染物去除研究豐碩，但於實際應用於現地整治時，成本效益與環境衝擊為材料選擇首要考量。實驗中使用的複合金屬是以零價鐵作為核心金屬，對一般使用零價鐵在進行整治時的限制進行改良，主要目的為減少零價鐵作為還原材料投入受污染水體，因與水體接觸造成零價鐵的迅速腐蝕現象並有效提升零價鐵在水體中的長效還原性。
本研究以化學還原方式自行製備鐵/鋁/鎳及鐵/鋁複合金屬，並進行材料元素分析、表面微觀分析及粒徑分析。因地殼及土壤金屬豐富度以鐵鋁為主，研究合成的複合金屬組成比值為鐵鋁比1：1，結果與實驗設計相符，且單一顆粒顆粒粒徑介於88-97奈米間，符合奈米級材料，能提高其反應面積。
實驗以批次試驗進行複合金屬對單一及兩種目標污染物去除的測試，得到初步測試結果，顯示複合金屬對兩種目標污染物皆有去除效果。但與國內外研究文獻相較之下，單一奈米零價鐵去除效果較佳，證實化學還原反應迅速，但應用於地下受污染含水層中，零價鐵易與環境中複雜成分反應而消耗，為了提高材料的長效性與控制現地呈現穩定厭氧環境，於是進行複合金屬的改良，包括改變金屬組成配比和加入酸洗程序。經酸洗液測試後，選擇以對環境衝擊小的檸檬酸進行測試，實驗配置3%、5%及10%檸檬酸溶液作為酸洗液，並添加鐵鋁比值為8：2的複合金屬配置成複合金屬懸浮液。再以此懸浮液進行六價鉻的去除實驗，結果在水中六價鉻濃度大於8000 毫克/升的環境下，金屬懸浮液對六價鉻還原效果為每克複合金屬可還原4.42克六價鉻，而在連續式補注六價鉻去除實驗中，顯示複合金屬懸浮液於重複添加污染物六價鉻的批次試驗下，每克複合金屬能還原0.875克六價鉻，在高濃度六價鉻環境下，其還原機制除物理吸附還原亦包含化學反應沉澱吸附；在連續污染物注入試驗中，可發現複合金屬在長時間試驗下可能與目標污染物以外之微量元素及水反應而消耗，但由單位材料反應結果顯示，不論在高濃度六價鉻(電鍍廢液槽)環境或是應用於現地環境之污染物持續注入實驗，複合金屬的污染物移除效率高。
本研究發現複合金屬在水質環境參數上具有提供酸鹼值緩衝的能力，並可使水體氧化還原電位呈還原態，有利於水中含氯有機物的還原脫氯及重金屬的還原，並進一步生成氫氧化物沉澱，有效移除水中重金屬。另外，在研究中也發現複合金屬可進行污染物去除的酸鹼值範圍較零價鐵廣泛，零價鐵一般而言適合在中性偏酸或酸性環境下進行污染物的去除，在鹼性條件下易在鐵表面生成氫氧化鐵而使還原性減弱，而實驗中複合金屬因在金屬表面有鋁層存在，在金屬表面易形成氫氧化鋁或氧化鋁層，在酸性或鹼性環境下易受強烈腐蝕作用洗去，使具強還原性的零價鋁層裸露以去除污染物，使複合金屬在水中酸鹼值4~9中皆能進行污染物的去除，大大提高了以複合金屬處理污染物的應用性。實驗結果顯示複合金屬顆粒在處理污染物後依然具有磁性，可利用電磁鐵等磁力作用進行回收，處理後的金屬顆粒由酸洗的方式進行複合金屬的再製及進行污染物的再去除。本研究結果可提供未來三氯乙烯或六價鉻污染場址整治技術的參考使用。

In this study, Fe-Al bimetallic nanoparticles (Fe-Al BNPs) was designed and applied to treat chromium and trichloroethylene (TCE) contaminated groundwater. Fe-Al BNPs was prepared by the chemical reduction process and the produced BNP had an averaged particle diameter of 88-97 nm.
Batch experiments were conducted to evaluate the efficiency of chromium and TCE removal efficiency with the addition of Fe-Al BNPs. The results show that Fe-Al BNPs can remove both target contaminants and the removal efficiencies for Cr6+ and TCE were 0.07g Fe-Al BNPs and 0.02g TCE/g Fe-Al BNPs, respectively, with the addition of 0.1 g/L of Fe-Al BNPs.
To improve the removal efficiency of Cr 6+ and TCE using Fe-Al BNPs, citric acid (10 wt%) was used to wash Fe-Al BNPs to form Fe-Al BNPs suspension. The suspension was applied for Cr6+ removal. Results of Cr6+ removal ratio was 4.42 g Cr6+/g Fe-Al BNPs with the addition of 1 g/L Fe-Al BNPs in the water contained approximately 8,.000 mg/L of chromium. Complete Cr removal efficiency was obtained with the continuous addition of 1 g/L Fe-Al BNPs.
Trivalent chromium (Cr3+) was detected in the aqueous phase during the Cr6+ removal process. X-Ray Diffractometer (XRD) analysis confirmed that Cr3+ was present on the surface of Fe-Al BNPs. The results of this study show that the application of BNPs can treat chromium and TCE-contaminated groundwater rapidly and effectively. In addition, the reproduced BNPs also had the potential to be reused in the treatment process.

誌謝 ................................................................................................................................................ i
中文摘要 ....................................................................................................................................... ii
Abstract ........................................................................................................................................iv
目錄 ............................................................................................................................................... v
圖目錄 ......................................................................................................................................... viii
表目錄 ........................................................................................................................................... x
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 ......................................................................................................................... 3
2.1地下水污染 ......................................................................................................................... 3
2.1.1含氯有機物污染概況 .................................................................................................. 3
2.1.2重金屬鉻污染概況 ...................................................................................................... 7
2.2污染物定義及特性 ............................................................................................................. 8
2.2.1三氯乙烯的性質與危害 .............................................................................................. 8
2.2.2鉻的性質與危害 ........................................................................................................ 10
2.2.3國內對兩種污染物現行管制標準 ............................................................................ 13
2.3污染物處理方法回顧 ....................................................................................................... 14
2.3.1水中含氯有機物去除之相關研究 ............................................................................ 14
2.3.2去除水中六價鉻污染之相關研究 ............................................................................ 17
2.4奈米零價鐵 ....................................................................................................................... 21
2.4.1奈米零價鐵的定義與特性 ........................................................................................ 21
2.4.2奈米零價鐵對污染物去除機制 ................................................................................ 22
2.4.3奈米零價鐵的改質 .................................................................................................... 25
2.5奈米複合金屬 ................................................................................................................... 26
2.5.1奈米複合金屬的定義與特性 .................................................................................... 26
2.5.2奈米複合金屬的製備 ................................................................................................ 27
2.5.3奈米複合金屬處理污染物研究回顧 ........................................................................ 31
2.6金屬在水溶液中之存在型態 ........................................................................................... 33
2.6.1鉻與水之 Eh-pH 平衡圖 ......................................................................................... 33
2.6.2鐵與水之 Eh-pH 平衡圖 ......................................................................................... 34
2.6.3鋁與水之 Eh-pH 平衡圖 ......................................................................................... 35
第三章 實驗設備與方法 ........................................................................................................... 36
3.1研究架構 ........................................................................................................................... 36
3.2研究流程 ........................................................................................................................... 37
3.2實驗材料與設備 ............................................................................................................... 38
3.2.1實驗材料 .................................................................................................................... 38
3.2.2實驗設備 .................................................................................................................... 38
3.2奈米金屬的製備 ............................................................................................................... 40
3.2.1奈米零價鐵的製備 .................................................................................................... 40
3.2.2奈米複合金屬的製備 ................................................................................................ 41
3.3污染物批次實驗 ............................................................................................................... 43
3.4複合金屬懸浮液處理Cr6+實驗 ....................................................................................... 45
3.5實驗分析方法 ................................................................................................................... 47
3.5.1金屬成分分析 ............................................................................................................ 47
3.5.2污染物分析 ................................................................................................................ 49
第四章 結果與討論 ................................................................................................................... 51
4.1複合金屬基本特性分析 ................................................................................................... 51
4.1.1鐵鋁鎳複合金屬 ........................................................................................................ 51
4.1.1鐵鋁複合金屬 ............................................................................................................ 56
4.2污染物批次實驗 ............................................................................................................... 61
4.2.1 三氯乙烯實驗組 ....................................................................................................... 62
4.2.2 複合污染物實驗組 ................................................................................................... 65
4.2.3批次試驗結果比較 .................................................................................................... 71
4.3 鐵鋁複合金屬的改良 ...................................................................................................... 72
4.3.1複合金屬金屬組成變更 ............................................................................................ 73
4.3.2酸洗液測試 ................................................................................................................ 74
4.4奈米金屬懸浮液處理高濃度Cr6+實驗 ........................................................................... 76
4.4.1檸檬酸組 .................................................................................................................... 77
4.4.2奈米零價鐵組 ............................................................................................................ 80
4.4.3複合金屬組 ................................................................................................................ 83
4.5奈米金屬處理連續補注Cr6+污染物實驗 ....................................................................... 86
4.5.1奈米零價鐵組 ............................................................................................................ 87
4.5.2複合金屬組 ................................................................................................................ 92
4.6 奈米金屬回收可行性 ...................................................................................................... 97
第五章 結論與建議 ................................................................................................................... 98
5.1結論 ................................................................................................................................... 98
5.2建議 ................................................................................................................................... 99
參考文獻 ................................................................................................................................... 100

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