臺灣博碩士論文加值系統

近來眾多研究報告指出，一般污水處理廠無法有效去除水中的新興污染物 (例如：咖啡因 (Caffeine)、雙酚A (Bisphenol A) 等)，若這些污水廠之放流水進入承受水體，並成為飲用水源，則會增加人體暴露在殘留新興污染物之機會。本研究之目的為：(1) 調查關切的藥物於某校園生活污水廠各處理單元之流佈及宿命；(2) 利用新穎管狀碳質/陶瓷複合膜結合同步電混凝/電過濾 (EC/EF) 程序處理含環境荷爾蒙及藥物之水樣，並評估最佳操作參數處理該校園生活污水之可行性；(3) 藉由Hermia 模式及阻力串聯模式來分析薄膜積垢現象及積垢阻力組成。
經由長期 (2010/09至2012/06) 每月份監測，於污水廠進流水中測得之藥物以先鋒黴素Ⅳ (Cefalexin)、咖啡因及磺胺甲噁唑 (Sulfamethoxazole) 具有較高檢測濃度和檢出率，最高檢測值分別為20,332.1 ng/L、30,490.2 ng/L及2,120.8 ng/L；檢出率則分別為72.7%、100%及100.0%。由單日間歇性監測結果可知，該校園生活污水廠中之上流式厭氧污泥反應池對於關切的藥物 (包括：1,1-二甲基雙胍鹽酸鹽 (1,1-Dimethylbiguanide hydrochloride)、先鋒黴素Ⅳ、四環素 (Tetracycline)、咖啡因、磺胺甲噁唑、紅黴素 (Erythromycin)、萘普生 (Naproxen)、三氯沙 (Triclosan)、布洛芬 (Ibuprofen)、待克菲那 (Diclofenac) 及吉非羅齊 (Gemfibrozil) 之平均去除率為46.03-61.12%，接觸氧化池為31.39-59.73%、終沉池為12.75-15.53%，而消毒處理單元為6.40-23.23%。
接著，利用反應曲面法來評估二種碳質/陶瓷複合膜搭配同步電混凝/電過濾程序處理含環境荷爾蒙及藥物之效能，碳/氧化鋁複合膜之聯立最佳操作參數為電場強度 45.71 V/cm及過濾壓差156.45 kPa；而碳纖維/碳/氧化鋁複合膜部分，最佳操作參數則為電場強度35.53 V/cm及過濾壓差330.59 kPa。
最後，經由Hermia阻塞模式及阻力串聯模式來探討碳質/陶瓷複合膜對於生活污水之阻塞情形，研究發現碳/氧化鋁複合膜主要以中等程度阻塞為主，而碳纖維/碳/氧化鋁複合膜則以濾餅阻塞現象為主；以阻力串聯模式來看，碳纖維/碳/氧化鋁複合膜之不可逆阻力較碳/氧化鋁複合膜小，而碳纖維/碳/氧化鋁複合膜過濾該校園生活污水於處理時間前10分鐘多以不可逆積垢為主，後續漸以可逆積垢為主。據此，碳纖維層確實具有提昇陶瓷複合膜之處理能力之功效。

In recent years, many studies have indicated that wastewater treatment plants (WWTPs) are incapable of removing emerging contaminants (e.g., caffeine and bisphenol A) effectively. Wastewater recycling increases the opportunity of emerging contaminants introduced into the drinking water systems and thus human exposure to emerging contaminants has escalated. The objectives of this research are three-fold: (1) to investigate the concentration variations and transport/spreading of pharmaceuticals in the water specimens obtained from major treatment units of the sewage treatment plant on a selected campus; (2) to treat emerging contaminants containing solutions by a combined treatment system of the simultaneous electrocoagulation/electrofiltration (EC/EF) process coupled with tubular carbonaceous/ceramic composite membrane and evaluate its feasibility of treating campus sewage; (3) to analyze the components of membrane fouling using Hermia’s model and resistances in series model.
Through long term monthly monitoring (from September 2010 to June 2012), cefalexin, caffeine, and sulfamethoxazole were detected at relativly higher concentrations (up to 20,332.1 ng/L, 30,490.2 ng/L, and 2,120.8 ng/L, respectively) and frequency detected (72.7%, 100% and 100%, respectively). The results of bi-hourly monitoring on a 24 h basis showed the ranges of removal efficiencies of concerned pharmaceuticals (including 1,1-dimethylbiguanide hydrochloride, cefalexin, tetracycline, caffeine, sulfamethoxazole, erythromycin, naproxen, triclosan, ibuprofen, diclofenac, and gemfibrozil) by the following treatment units of the selected campus WWTP: (1) up-flow anaerobic sludge bed reactor: 46.03-61.12%; (2) contact aeration unit: 31.39-59.73%; (3) secondary sedimentation tank: 12.75-15.53%, and (4) disinfection unit: 6.04-23.23%.
Furthermore, the experimental design using the response surface methodology (RSM) was employed to evaluate the performance of the EC/EF process in conjunction with tubular carbonaceous/ceramic composite membrane in removing emerging contaminants from aqueous solutions. The resulting optimal conditions for simultaneous optimization for the tubular carbon/alumina composite membrane (TCACM) were determined to be the electric field strength of 45.71 V/cm and transmembrane pressure of 156.45 kPa. The corresponding optimal conditions for the tubular carbon fibers/carbon/alumina composite membrane (TCCACM) were 35.53 V/cm and 330.59 kPa, respectively.
Finally, the membrane fouling was analyzed using Hermia’s model and resistances in series model for the selected campus sewage. Based on Hermia’s model, it was found that the major fouling mechanism for TCACM was intermediate blocking, whereas cake formation for TCCACM. Based on resistances in series model, the results showed that TCCACM had lesser irreversible resistance component (Rirr) than that of TCACM. When using TCCACM to treat the selected campus sewage, fouling in the first 10 min was mainly irreversible, then gradually became reversible afterward. Accordingly, the carbon fiber layer on TCCACM indeed could enhance the treatment performance as compared with TCACM.

聲明切結書 i
謝誌 ii
摘要 iiii
Abstract iv
目錄 v
圖目錄 xi
表目錄 xv
照片目錄 xix
第一章 前言 1
1.1 研究緣起 1
1.2 研究目的 4
1.3 研究內容與架構 5
第二章 文獻回顧 8
2.1 環境荷爾蒙與藥物及個人保健用品之特性來源 8
2.1.1 水體中之新興污染物之流佈 10
2.1.2 新興污染物常見之處理方式 17
2.1.3 環境荷爾蒙及藥物 20
2.1.4 標的污染物之物化特性 23
2.2 薄膜處理程序 26
2.2.1 薄膜分離程序 26
2.2.2 薄膜組件之形式 28
2.2.3 薄膜之材質 30
2.2.4 薄膜過濾之操作形式 31
2.3 薄膜過濾機制 33
2.3.1 去除率影響因子 36
2.3.1.1 薄膜之物化特性 36
2.3.1.2 新興污染物之物化特性 37
2.3.1.3 水質特性 38
2.4 電混凝/電過濾程序 40
2.4.1 電混凝 40
2.4.2 掃流電過濾 43
2.4.3 同步電混凝/電過濾程序 46
2.5 薄膜積垢 48
2.5.1 薄膜積垢機制 48
2.5.2 薄膜積垢阻力分析 52
2.6 實驗設計 56
2.6.1 迴歸模型 56
2.6.2 中央合成設計 59
2.6.3 迴歸模型的配適性 61
2.6.4 聯立最佳化技術 64
2.6.5 反應曲面法於環工領域之應用 68
第三章 實驗材料、設備與方法 70
3.1 實驗材料 70
3.1.1 水樣來源 70
3.1.2 材料與試劑 71
3.2 實驗設備 73
3.2.1化學氣相沉積設備 73
3.2.2 蒸氣壓氣體滲透偵測裝置 73
3.2.3 同步電混凝/電過濾模組處理系統 73
3.2.4 其他設備及儀器 75
3.3 實驗方法 77
3.3.1 管狀碳/氧化鋁及碳纖維/碳/氧化鋁複合膜製備程序 77
3.3.2 管狀碳/氧化鋁及碳纖維/碳/氧化鋁複合膜之顯微結構觀測與薄膜孔徑分佈測定 78
3.3.3 同步電混凝/電過濾處理系統之操作 79
3.3.4 含環境荷爾蒙及藥物之模擬水樣配製 81
3.3.5 水樣及濾液品質分析方法 81
3.3.6 實驗參數設計 85
第四章 結果與討論 88
4.1 管狀陶瓷複合膜之特性分析 88
4.1.1 複合膜表面與截面顯微結構 88
4.1.2 管狀無機複合膜孔徑分布 90
4.2 藥物在某校園生活污水廠各處理單元之流佈探討 92
4.2.1 長期性每月採樣分析 92
4.2.1.1 進流水之流佈探討 92
4.2.1.2 進流水、放流水之測值與檢出率 .96
4.2.2 單日間歇性採樣分析 101
4.3 同步電混凝/電過濾程序處理含環境荷爾蒙及藥物水樣與實際生活污水 109
4.3.1 管狀碳/氧化鋁複合膜處理含環境荷爾蒙及藥物之水樣 109
4.3.1.1 實驗設計參數對環境荷爾蒙及藥物去除成效之影響 109
4.3.1.2 反應曲面法之變異數分析 114
4.3.1.3 最佳去除環境荷爾蒙及藥物之參數探討 121
4.3.1.4 電場強度及過濾壓差對濾液通量的影響 125
4.3.1.5 臨界電場強度探討 128
4.3.2 管狀碳纖維/碳/氧化鋁複合膜處理含環境荷爾蒙及藥物之水樣 130
4.3.2.1 實驗設計參數對環境荷爾蒙及藥物去除成效之影響 130
4.3.2.2 反應曲面法之變異數分析 131
4.3.2.3 最佳去除環境荷爾蒙及藥物之參數探討 138
4.3.2.4 電場強度及過濾壓差對濾液通量的影響 143
4.3.2.5 臨界電場強度探討 145
4.3.3 整體實驗之評估 147
4.3.3.1 最佳操作條件應用於實際生活污水 147
4.4 管狀碳質/陶瓷複合膜之薄膜積垢分析 149
4.4.1 Hermia Model評估薄膜阻塞機制 149
4.4.2 薄膜積垢阻力分析 153
第五章 結論與建議 158
5.1 結論 158
5.2 建議 160
參考文獻 161
附錄......... 161
附表1 2010年9月至2011年8月期間關切的藥物於某校園生活污水廠進流水之濃度分布情況 (ng/L) 190
附表2 2011年8月至2012年6月期間關切的藥物於某校園生活污水廠進流水之濃度分布情況 (ng/L) 191
附表3碳/氧化鋁複合膜搭配同步電混凝/電過濾程序去除水中之環境荷爾蒙及藥物之實驗數據 192
附表3碳/氧化鋁複合膜搭配同步電混凝/電過濾程序去除水中之環境荷爾蒙及藥物之實驗數據 (續) 193
附表4 碳纖維/碳/氧化鋁複合膜搭配同步電混凝/電過濾程序去除水中之環境荷爾蒙及藥物之實驗數據 194
附表4 碳纖維/碳/氧化鋁複合膜搭配同步電混凝/電過濾程序去除水中之環境荷爾蒙及藥物之實驗數據 (續) 195
附表5 達到95%信心水準之最小F值 196
碩士在學期間發表之學術論文 197

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