國內用水約有四分之一來自地下水，然而近年工業區或廢棄物處置場地下水受含氯有機溶劑污染事件頻傳，其中三氯乙烯(trichloroethene, TCE)具有生物累積性與致癌性危害。許多研究指出組合式薄膜程序(hybrid membrane process)可降低阻塞並提昇污染物去除效率。本研究以纖維過濾(fiber filtration, FF)為奈米過濾(nanofiltration, NF)的前處理，以FF+NF組合程序去除地下水中懸浮固體(suspended solid, SS)、TCE及其它污染物，評估經過薄膜組合程序處理後滲透液作為再生水之可行性。首先以人工配製含高嶺土之TCE溶液為實驗對象，測量FF去除懸浮固體與降低濁度之最佳濾速，再以微過濾(microfiltration, MF)、超過濾(ultrafiltration, UF)及奈米過濾測試含TCE溶液之去除率與TCE對薄膜通量之影響。接著評估FF+NF組合程序處理受TCE污染地下水作為再生水之可行性。最後以掃描式電子顯微鏡(scanning electron microscope, SEM)與能量散射光譜儀(energy dispersive spectroscope, EDS)觀察膜面受污染物破壞程度，以及三維螢光激發發射矩陣(3-D excitation emission fluorescence matrix, EEFM)與紫外光UV分析膜面有機阻塞之潛勢。研究結果顯示，FF最佳濾速為15.3 m/hr，可攔截TCE與SS而且去除率分別為80與60%。MF與UF去除TCE以篩除(sieving)為機制，NF去除TCE以篩除與靜電排斥(electrostatic repulsion)為機制。三種薄膜以NF去除1 mg/L之TCE效果最佳去除率可達98.2%。NF處理低濃度TCE去除率較高，可能膜孔收縮所造成；而高濃度TCE會破壞NF膜面，使膜孔變大導致TCE去除率較差。FF+NF組合程序對SS、硫酸鹽及總硬度去除率分別提昇至99.8%、98.7%及98.7%；而添加TCE之地下水相較於未添加之地下水，經過薄膜組合程序TCE去除率可從72.9%提昇至98.9%。TCE通過薄膜通量較清水通量低，應為TCE累積於膜面造成阻力。高濃度TCE使膜孔變大導致濃縮效果降低與通量增加。FF可去除SS降低薄膜阻塞，有效減緩46%之NF通量降低。實驗以5 mg/L之TCE通過NF，再以甲醇沖洗膜面，結果濃縮液TCE約1.1 mg/L，證明TCE會殘留於膜面。地下水中顆粒之界達電位較低，顆粒電雙層壓縮傾向聚集；經過薄膜組合程序處理後滲透液中顆粒之界達電位變高，顆粒排斥力大而穩定性高。經過SEM分析，發現TCE會造成膜面破壞；地下水中重金屬會造成膜面阻塞。經過EEFM、非揮發性溶解有機碳(non-purgable dissolved organic carbon, NPDOC)及紫外光(UV254)分析，發現地下水含有腐植酸(humic acid, HA)與溶解性微生物副產物(soluble microbial by-product, SMP)；經過FF處理後，HA與SMP可能會吸附於濾材；或濾材表面附著生物膜之胞外聚合物(extracellular polymeric substances, EPS)被沖洗出，另可能為纖維濾材表面之可能被沖洗出造成NPDOC增加；經過FF+NF組合程序處理後，HA被NF攔截去除，SMP吸附於膜孔造成有機阻塞或被沖洗出。由本研究結果可知，經過FF前處理可改善通量降低，高濃度TCE會破壞膜面使分離效率降低。受TCE污染地下水經過FF+NF組合程序處理後，滲透液TCE濃度可符合第二類地下水污染物管制標準，其他水質項目也符合B類與C類之再生水標準，可作為工業冷卻與都市澆灌用水。

In Taiwan, more than 25% of all water uses comes from groundwater, and thus groundwater is a very valuable water resource for both domestic and industrial uses. However, groundwater at many existing former industrial sites and disposal areas was contaminated by halogenated organic compounds that were released into the environment. The chlorinated solvent trichloroethene (TCE) is one of the most ubiquitous of these compounds. In this laboratory-scale feasibility study, a hybrid two-stage process combining fiber filtration (FF) and nanofiltration (NF) was applied to remove to suspended solids (SS) and TCE from contaminated groundwater for water purification. In this study, a man-made kaolin solution was used to simulate groundwater purification using FF system. Then, microfiltration (MF), ultrafiltration (UF), and NF systems were applied for TCE removal. The hybrid membrane process using FF and NF units was used to evaluate the feasibility on TCE removal. The scanning electron microscope (SEM) and energy dispersive spectroscope (EDS) were used to investigate membrane morphology and structure after use. A 3-D excitation emission fluorescence matrix (EEFM) was used to evaluate the potential of membrane organic fouling. Results show that the optimization filtration velocity of FF was 15.3 m/hr, and the observed TCE and SS removal efficiencies were 80% and 60%, respectively. Removal mechanisms for MF and UF were mainly sieving, and the removal mechanism for NF was mainly electrostatic repulsion. Results indicate that NF had the highest TCE removal efficiency (98.2%). When initial TCE concentration was 1 mg/L, NF membrane pore might shrink caused increased TCE removal (rejection). When TCE concentration was higher 1 mg/L, membrane damage and pore enlargement was observed with decreased TCE removal efficiency. The observed SS, sulfate, and hardness removal efficiencies were 99.8%, 98.7%, and 98.7% respectively, when FF and NF hybrid process was used. Higher TCE concentration might enlarge membrane pore, which caused decreased membrane separation and increased flux. Approximately 46% of flux drop was observed when NF was used alone compared to the hybrid membrane process using FF as the first treatment stage. Membrane analyses show that residual TCE was adsorbed on the membrane. Low zeta potential of groundwater was observed due to the compressed electric double layer, which caused aggregation of particle. High zeta potential of permeate was due to the particle dispersive through hybrid process. Results from SEM analysis show that membrane morphology was damaged by TCE, and heavy metal in groundwater deposited on membrane. Results of EEFM analysis indicate that groundwater contained humic acid (HA) and soluble microbial by-product (SMP). HA and SMP might be adsorbed on fiber filter, and extracellular polymeric substances (EPS) that attached on fiber filter might be washed out. The organic powders on the surface of the fiber filter might be washed out causing the increased in NPDOC concentrations. Humic acid could be removed through NF process, and SMP might be adsorbed in membrane pore caused organic fouling, and SMP might be washed out after treatment by the FF+NF hybrid process. Results indicate that FF as pre-treatment can maintain higher flux. Higher TCE concentration caused membrane destruction and decreased membrane separation. TCE contaminated groundwater can be affectively treated by the hybrid membrane system to meet the groundwater standard and reclaimed water standard. Reclaimed water could be used for industrial cooling water and irrigation purposes.

誌謝 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
1.2 研究目的 2
第二章 文獻回顧 3
2.1 地下水受含氯有機物污染概況 3
2.1.1 含氯有機物污染來源 3
2.1.2 三氯乙烯特性與危害 4
2.2 水回收再利用現況 7
2.2.1 水再生之用途 7
2.2.2 國內水再生利用現況 7
2.3 纖維過濾 9
2.3.1 纖維過濾之構造與應用 9
2.3.2 纖維過濾之優缺點 9
2.4 薄膜程序 10
2.4.1 驅動方式 10
2.4.2 材質與特性 11
2.4.3 分離之種類 12
2.4.4 組件與型式 15
2.4.5 過濾與操作參數 16
2.5 薄膜分離常見問題與控制 18
2.5.1 薄膜阻塞 18
2.5.2 濃度極化 19
2.5.3 膜面性質改變 20
2.5.4 進流水前處理 21
2.5.5 薄膜清洗 21
2.6 膜面與水中有無機物分析之應用 22
2.6.1 界達電位 22
2.6.2 掃描式電子顯微鏡 23
2.6.3 三維螢光激發發射矩陣 24
2.6.4 非揮發溶解有機碳與紫外光 26
第三章 實驗材料、設備及研究方法 27
3.1 研究流程 27
3.2 實驗藥品、材料及分析儀器 29
3.2.1 實驗藥品 29
3.2.2 實驗材料 30
3.2.3 分析儀器 31
3.3 實驗方法與設備 31
3.3.1 纖維過濾試驗 31
3.3.2 薄膜模組試驗 34
3.3.3 薄膜組合程序 39
3.4 分析項目及方法 40
3.4.1 水質參數分析 40
3.4.2 薄膜通量 41
3.4.3 膜面三氯乙烯濃縮分析 41
3.4.4 氣相層析儀-電子捕捉器分析 41
3.4.5 界達電位分析 42
3.4.6 掃描式電子顯微鏡與能量散射光譜儀分析 42
3.4.7 三維螢光激光放射矩陣分析 42
3.4.8 紫外光分析 43
第四章 結果與討論 44
4.1 地下水水質特性 44
4.2 纖維過濾水質探討 46
4.2.1 最佳操作濾速測試 46
4.2.2 地下水污染物經過纖維過濾處理成效 47
4.3 薄膜滲透液探討 51
4.3.1 不同薄膜對三氯乙烯去除效果 51
4.3.2 膜面耐受性測試 53
4.3.3 膜面三氯乙烯濃縮試驗 55
4.4 薄膜組合程序處理地下水污染物之成效 56
4.5 薄膜通量與阻塞分析 63
4.5.1 不同薄膜之去離子水通量比較 63
4.5.2 不同薄膜添加三氯乙烯通量比較 64
4.5.3 不同三氯乙烯濃度對奈米過濾通量影響 65
4.5.4 纖維過濾改善通量降低與減緩阻塞 66
4.6 膜面阻塞探討 67
4.6.1 地下水與滲透液中顆粒之界達電位探討 67
4.6.2 三氯乙烯及地下水成分對膜面的影響 68
4.6.3 地下水及滲透液之有機物探討 74
4.7 薄膜清洗與膜孔殘留物探討 82
4.8 薄膜組合程序經濟效益評估 83
第五章 結論與建議 85
5.1 結論 85
5.2 建議 87
參考文獻 88
縮寫表 104
附錄一 106
附錄二 108

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