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論文名稱 Title |
以電透析結合薄膜技術處理及回收含過氯酸鹽之地下水 Using electrodialysis and membrane hybrid system to treat and recover perchlorate-contaminated groundwater |
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系所名稱 Department |
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畢業學年期 Year, semester |
語文別 Language |
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學位類別 Degree |
頁數 Number of pages |
116 |
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研究生 Author |
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指導教授 Advisor |
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召集委員 Convenor |
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口試委員 Advisory Committee |
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口試日期 Date of Exam |
2016-07-19 |
繳交日期 Date of Submission |
2016-08-22 |
關鍵字 Keywords |
電透析、地下水、水回收、過氯酸鹽、薄膜 electrodialysis reversal, water reclaim, perchlorate, membrane, groundwater |
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統計 Statistics |
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中文摘要 |
過氯酸鹽(perchlorate, ClO4-)是一種具高氧化力、高水溶性以及低黏滯性之物質,長期被廣泛用於煙火、爆炸物、火箭推進劑等製造之成分。此外,ClO4-在水中可穩定且長久存在,並容易隨地下水流動而擴散,造成大範圍ClO4-污染之情形。人體若攝取過量的過氯酸鹽,將可能影響甲狀腺之正常功能,進而抑制人體吸收碘的能力。本研究以具倒極清洗薄垢功能之電透析(electrodialysis reversal, EDR)結合逆滲透(reverse osmosis, RO)形成組合式程序(EDR+RO),進行地下水處理及回收之研究。試驗結果顯示,EDR系統會因電壓(V)提升,使電動力驅動而加速離子的遷移,並在符合經濟效益範圍內,EDR於40 V電壓操作時有最佳之ClO4-去除率(94.5%)與最短之去除時間(2.5 hr),其中本研究比較RO直流(one through)及迴流(reflux)操作對滲透液水質淨化程度,結果顯示直流操作可再將ClO4-處理至0.02 mg/L以下,另迴流操作會使濃縮液中的ClO4-會不斷累積於薄膜表面(membrane proe),使得滲透液水質變差,但淨化後之水質仍可符合澆灌用水規範。 經現地採集地下水測試,當EDR+RO直流系統可將ClO4-移除99.9%以上,而水中其他離子(如TH、Alk、Cl-、NO3-、SO42-、ClO4-、重金屬)亦能有效濃縮,且移除率皆大於95%,另迴流操作亦可將過氯酸鹽移除98.2%,但整體水中離子移除率低於直流操作,同樣結果證實迴流提濃水中離子及ClO4-等污染物,造成膜孔累積並形成積垢。同時本研究為了瞭解EDR+RO濃縮水中高濃度ClO4-去化,嘗試透過零價金屬Fe0、Al0針對ClO4-之還原特性,試驗結果兩者去除率分別為13.7%與30.8%,顯示化學還原法具處理ClO4-濃縮液之潛力。 膜面無機物積垢試驗,據掃描式電子顯微鏡(scanning electron microscope, SEM)與能量散射光譜儀(energy dispersive spectrometer, EDS)分析發現,EDR處理含過氯酸鹽地下水後,其陽離子交換膜具有之強酸性官能基為磺酸基(SO3H),電極與電流之作用,使陽離子交換膜之酸性官能基被電解出,導致離子交換膜上之含硫量增加,而膜面也發現有碳酸鈣(CaCO3)之沉積物。而RO膜之SEM-EDS膜面分析發現,膜上重金屬沉積物(鉬、鎂、砷、鉀)之種類較多。有機物積垢試驗,經過三維螢光激發發射矩陣(3-D excitation-emission fluorescence matrix, EEFM)分析發現,現地地下水以第II類芳香型類蛋白質(aromatic protein, AP)及第IV類溶解性微生物代謝物質(Soluble microbial by-product-like, SMP)之有機物比例最多,含ClO4-地下水經EDR處理後,濃縮水中蛋白質(AP)螢光波峰強度較淡水略為增強,證實EDR對於水中有機物分離效果有限,再經EDR+RO處理後,滲透液中第II類芳香型類蛋白質(AP)與溶解性微生物代謝物質(SMP)含量均小於進流水(EDR出流淡水),顯示RO膜可吸附及攔除低分子量有機物。 本研究以EDR結合RO系統處理含ClO4-之地下水,結果呈現,每噸水處理費用為23.74元,且EDR+RO直流操作可有效將10 mg/L之過氯酸鹽處理至偵測極限(0.02 mg/L)以下,可接近美國飲用水法規標準(15 μg/L),其他水質項目亦可符合澆灌用水水質標準與注入地下水體水質標準及有害健康物質之種類、限值,可作為澆灌用水與注入地下水之再生水用途。另地下水中ClO4-原料及鹽類於EDR中因電解而產生鹽酸(HCl)及氯離子(Cl-)等中間產物,使EDR出流水質呈現酸性,對後續RO處理應有抑制氫氧化物或積垢物累積之效果,故以EDR結合RO之技術處理低污染地下水作為再生水,較傳統廢水處理程序具有其可行性及優勢。 |
Abstract |
Perchlorate (ClO4-) is a high oxidizing, high water solubility and low viscosity material, which is commonly used as an oxidizer in fireworks, explosives rocket propellants, and other manufacturing. In addition, perchlorate can be stably present in groundwater for a long term, and can easily diffuse with the groundwater flow and cause a large-scale pollution. Because perchlorate has been linked to its negative influence on the thyroid gland, human will be inhibit their ability to absorb iodine if intaking excessive perchlorate. To solve this problem, a hybrid electrodialysis and reversal-reverse osmosis process (EDR + RO) was carried out to treat and recycle perchlorate-contaminated groundwater in this study. The results show that voltage (V) played an important role in EDR performance, which enhanced the migration of ions in water with increased voltage. Up to 94.5% of ClO4- could be removed in 2.5 hours of operation at 40. Effluent from the EDR unit was passed through the RO unit and results show that the perchlorate was desalinated to below 0.02 mg/L after the RO treatment. Although the water quality was significantly improved, however, it could barely meet the standard of irrigation water quality. In this study, site groundwater was used for the feasibility study. Up to 99.9% of ClO4- can be removed via the two stage system (EDR + RO) system. More than 95% of other ions in water (e.g., Cl-, NO3-, SO42-, ClO4-, heavy metals) were also concentrated and removed via the EDR system. Effluents from the EDR system could be further treated via the followed RO system. More than 98% of ClO4- and other ions were removed after the RO unit. This results also indicate that perchlorate and other ions in water accumulated in the membrane pores and formed fouling. To solve perchlorate concentrate after EDR + RO desalination, zero-valent iron (Fe0) and zero-valent aluminum (Al0) were used to reduce the concentrates via the chemical reduction process. Results show that approximately 13.7% and 30.8% of ClO4- could be reduced by Fe0 and Al0, respectively. It indicates that chemical reduction process is a potential method to treat perchlorate concentrate. Results from scanning electron microscope (SEM) and energy dispersive spectroscopy (EDS) analyses show that the strong acidic functional group [sulfonic acid group (SO3H)] on the EDR cation exchange membrane was electrolyzed after EDR+RO treatment. This demonstrates that the contents of sulfur accumulated on the ion-exchange membrane. Moreover, calcium carbonate (CaCO3) sediments were observed on the membrane pores. The SEM-EDS analysis results show that heavy metals (such as molybdenum, magnesium, arsenic, potassium) deposited on the RO membrane. Results from the 3-D excitation-emission fluorescence matrix (EEFM) show that the most proportion of organic matter in groundwater was the type II of aromatic protein (AP) and the type IV of soluble microbial by-product-like (SMP). This indicates that the EDR treatment had less effect on organic compound separation. After the treatment of EDR and RO units, AP and SMP contents in filtrate were lower than feed water (the desalination water of EDR). Therefore, the RO membrane can adsorb and block the organics with low molecular weights. Results indicate that the two two-stage system could effectively treat perchlorate-contaminated groundwater to below 0.02 mg/L, and the estimated cost for groundwater treatment was about NT$23.74/ton of groundwater (with initial perchlorate concentration of 10 mg/L). The treated groundwater could meet the irrigation standard and subsurface injection standard. Moreover, the system could electrolyzed perchlorate and generate hydrochloric acid (HCl) and chlorine ions (Cl-), which resulted in the acidified effluents. This could inhibit the hydroxide production and prevent the fouling on the RO membrane. Results indicate that using the hybrid (EDR+RO) system is a feasible and effective method for the treatment and reuse of perchlorate-contaminated groundwater. |
目次 Table of Contents |
誌謝 i 摘要 ii Abstract iv 目錄 vi 圖目錄 ix 表目錄 xi 第一章 前言 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 過氯酸鹽 4 2.1.1 地下水中過氯酸鹽之來源與應用 5 2.1.2 過氯酸鹽之特性與危害 6 2.1.3 過氯酸鹽之處理技術 9 2.2 電透析技術 13 2.2.1 電透析(electrodialysis, ED) 13 2.2.2 倒極式電透析(electrodialysis reversal, EDR) 14 2.2.3 離子交換膜之種類與特性 14 2.2.4 離子在膜中遷移之作用 16 2.2.5 ED/EDR系統之操作與影響 17 2.3 薄膜過濾技術 19 2.3.1 薄膜過濾類型 19 2.3.2 薄膜驅動方式與操作參數 21 2.3.3 薄膜材質與特性 23 2.3.4 薄膜組件與形式 23 2.3.5逆滲透系統之操作與影響 25 2.4 以EDR+RO組合程序進行水回收再利用 26 2.4.1 水再生用途 26 2.4.2 國內水再生現況 27 2.4.3 EDR與RO技術之比較 28 2.4.4 EDR+RO組合程序之應用 29 2.5 膜面與水中有無機物分析之應用 30 2.5.1 掃描式電子顯微鏡 30 2.5.2 有機物之來源與分類 31 2.5.3 三維螢光激發發射矩陣 31 第三章 實驗方法與設備 33 3.1 研究架構 33 3.2 實驗藥品及材料 35 3.2.1 實驗藥品 35 3.2.2 實驗材料 35 3.2.3 分析儀器 36 3.3 實驗方法與設備 36 3.3.1 EDR試驗 36 3.3.2 RO試驗 40 3.4 組合程序試驗 43 3.5 分析項目及方法 45 3.5.1 水質項目分析 45 3.5.2 離子層析儀分析 46 3.5.3 掃描式電子顯微鏡與能量散射光譜儀分析 46 3.5.4 螢光激發發射光譜分析 46 第四章 結果與討論 48 4.1 地下水水質特性 48 4.2 電透析處理水質探討 50 4.2.1 最佳操作參數測試 50 4.2.2 過氯酸鹽中間產物生成與解離機制 55 4.2.3 地下水污染物經過EDR處理成效 56 4.3 薄膜滲透液探討 59 4.3.1 最佳操作參數測試 59 4.3.2 過氯酸鹽經過RO薄膜之處理成效 59 4.4 電透析結合薄膜技術處理地下水污染之成效 62 4.4.1 地下水經EDR之處理成效 62 4.4.2 地下水經EDR+RO直流效應之處理成效 66 4.4.3 地下水經EDR+RO迴流效應之處理成效 69 4.5 膜面阻塞探討 72 4.5.1 含過氯酸鹽地下水對膜面之影響 72 4.5.2 地下水及滲透液之有機物探討 77 4.6 過氯酸鹽濃水去化試驗 82 4.7 經濟效益評估 83 第五章 結論與建議 84 5.1 結論 84 5.2 建議 86 參考文獻 87 附錄一 101 |
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