本研究工作主要針對台灣南部某校園生活污水處理廠進/放流水、自來水及飲水機出流水中關切之8種鄰苯二甲酸酯類、雙酚A、壬基酚、18種抗生素類藥物及10種非抗生素類藥物等新興污染物進行長期的監測，並使用具有過濾及吸附功能之碳質/氧化鋁複合膜結合同步電混凝/電過濾程序應用在水中新興污染物之去除。根據該校園水質調查結果，可以發現前述所有水體中通常至少含有3種以上之新興污染物，其中，生活污水中以先鋒黴素（Cephalexin）與咖啡因（Caffeine）為平均濃度最高者，其最高濃度分別可達5,199 ng/L及915 ng/L；而自來水及飲水機出流水則以鄰苯二甲酸二丁酯（DnBP）、鄰苯二甲酸二(2-乙基己基)酯（DEHP）及鄰苯二甲酸二異壬酯（DiNP）最為常見，平均濃度介於16-93 ng/L。
本研究亦利用4種管狀濾膜（包括：氧化鋁陶瓷膜、疏水性改質氧化鋁陶瓷膜、二氧化鈦/氧化鋁複合膜及碳質/氧化鋁複合膜），針對含關切新興污染物之模擬水樣進行相關去除機制的探討，試驗結果指出，微過濾陶瓷膜經疏水性改質後，其對模擬水樣中DnBP、DEHP及DiNP等化合物之去除效率可從10%以下提升至10-20%之間；另外，碳質/氧化鋁複合膜其表層奈米碳纖維確實能提升水中新興污染物之去除成效，相較於孔徑相近之二氧化鈦/氧化鋁超過濾複合膜，對於水中Caffeine去除率可從46%提升至69%。
同步電混凝/電過濾（EC/EF）試驗部分，主要針對不同水體中關切的新興污染物進行試驗：以模擬水樣而言，水中關切化合物之去除率皆可超過60%，主要之去除機制來自於電過濾、電混凝及碳吸附效應；於選定的某校園生活污水廠進流水方面，試驗發現天然有機物質（NOM）之存在對生活污水中關切化合物之去除具有正面的影響，加上電混凝及電過濾效應之作用，使得生活污水中標的化合物之去除率皆能超過75%，最高去除率者為Cephalexin（96%）；選定的某校園自來水部分，其處理機制則以電混凝及碳吸附效應為主，而自來水中關切化合物之去除率主要介於67-92%之間。最後，阻力串聯模式分析結果發現，薄膜處理結合EC/EF程序，可以有效降低其不可逆之積垢，提高薄膜之耐用性。

This study investigated the occurrence and removal efficiencies of 8 phthalate esters, Bisphenol A, Nonylphenol, 18 antibiotics, and 10 non-antibiotics present in the influent of a sewage treatment plant (STP), tap water, and drinking fountain water on a selected campus in southern Taiwan. To this end, a monitoring program was conducted and a novel laboratory-prepared tubular carbonaceous/alumina composite membrane (TCACM) was incorporated into the simultaneous electrocoagulation and electrofiltration (EC/EF) treatment module to remove the emerging contaminants (ECs) from water samples. The monitoring results showed that at least three kinds of ECs present in each of the abovementioned aqueous solutions. It was found that the influent of selected campus STP contained cephalexin and caffeine with concentrations up to 5199 ng/L and 915 ng/L, respectively. Three PAEs (i.e., di-n-butyl phthalate (DnBP), di-(2-ethylhexyl) phthalate (DEHP), and di-iso-nonyl phthalate (DiNP)) were usually detected in tap water and drinking fountain water of concern with average concentrations ranging from 16 to 93 ng/L.
Four kinds of lab-perpared membrane, including tubular alumina membrane (TAM), tubular hydrophobically modified TAM, tubular titania/alumina composite membrane (TTACM), and TCACM, were used to investigate relevant removal mechanisms for ECs of concern in model solution. It was found that the removal efficiencies were significantly higher (10-20%) for the tubular hydrophobically modified TAM as compared with TAM. When carbon nanofibers (CNFs) layer was grown on TAM, this membrane would yield a much greater removal efficiency as compared with TTACM, for example, the removal efficiency of caffeine could increase from 46% to 69%.
The test results of the EC/EF process coupled with the TCACMs were also discussed. In model solution, removal efficiencies of over 60% were obtained for all ECs of concern. The synergistic effect of electrocoagulation and electrofiltration was considered as a probable mechanism. For the influent of campus STP, the said synergistic effect yielded the removal efficiencies up to 93% for DnBP, 95% for DEHP, 92% for DiNP, 96% for cephalexin, 95% for ciprofloxacin, 95% for caffeine, and 90% for sulfamethoxazole. Additionally, natural organic matter (NOM) was believed to enhance the removal of ECs from the influent of campus STP. It was also found that 69-72% removal efficiencies of ECs could be obtained in treatment tests of tap water. Effects of electrocoagulation and adsorption of CNFs are believed to be responsible for this finding.
According to the analysis based on the resistance in series model, the EC/EF process coupled with the TCACM yielded a lower irreversible resistance of membrane, resulting in a longer membrane life.

論文審定書 i
聲明切結書 ii
謝誌 iii
摘要 iv
Abstract vi
目錄 viii
圖目錄 xiii
表目錄 xvii
照片目錄 xxi
第一章 前言 1
1.1 研究緣起 1
1.2 研究目的 3
1.3 研究項目 6
第二章 文獻回顧 11
2.1 新興污染物之流布及去除 11
2.1.1 水體中關切之新興污染物的流布 11
2.1.2 關切的新興污染物常見之處理技術 18
2.1.3 關切之新興污染物其相關資訊 24
2.2 薄膜單元 31
2.2.1 薄膜定義與特性 31
2.2.2 薄膜分離程序 32
2.2.3 薄膜組件之形式 34
2.2.4 無機膜之特性 36
2.3 同步電混凝/電過濾程序 38
2.3.1 電混凝之應用 38
2.3.2 掃流電過濾之應用 40
2.3.3 同步電混凝/電過濾程序 44
2.4 變異數分析 47
2.5 薄膜阻力串聯模式 54
第三章 實驗材料、設備與方法 56
3.1 實驗材料 56
3.1.1 生活污水廠進流水及放流水來源 56
3.1.2 自來水及飲水機出流水來源 57
3.1.3 管狀氧化鋁陶瓷膜及其複合膜 57
3.1.4 其他材料與試藥 59
3.2 實驗設備 62
3.2.1 化學氣相沉積設備 62
3.2.2 同步電混凝/電過濾模組 62
3.2.3 蒸氣壓氣體滲透偵測裝置 64
3.2.4 其他實驗設備及儀器 64
3.3管狀氧化鋁陶瓷膜及其複合膜之製備 67
3.3.1 管狀氧化鋁陶瓷膜 67
3.3.2 管狀二氧化鈦/氧化鋁複合膜 68
3.3.3 管狀碳質/氧化鋁複合膜 69
3.4 實驗方法 70
3.4.1 含關切新興污染之模擬水樣配製 70
3.4.2 水樣及濾液品質分析方法 70
3.4.3 掃流過濾試驗 74
3.4.4 同步電混凝/電過濾試驗 77
3.5 實驗設計（AVOVA的應用）78
第四章 結果與討論 81
4.1 關切的新興污染物於選定的某校園生活污水廠進/放流水、自來水及飲水機出流水之調查與探討 81
4.1.1生活污水廠進流水及放流水 81
4.1.2 自來水及飲水機出流水 92
4.1.3 綜合探討 100
4.2 管狀陶瓷膜及其複合膜之特性分析 104
4.2.1 表面疏水性改質 104
4.2.2 顯微結構觀測 107
4.2.3 孔徑分布測定 116
4.3 管狀陶瓷膜及其複合膜去除水中新興污染物之探討 118
4.3.1 尺寸排除效應 119
4.3.2 疏水性效應 121
4.3.3 碳吸附效應 124
4.3.4 綜合探討 134
4.4 管狀碳質/氧化鋁複合膜結合同步電混凝/電過濾程序去除 水中新興污染物之探討 137
4.4.1 模擬水樣 137
4.4.2 選定的某校園生活污水處理廠進流水 147
4.4.3 選定的某校園自來水 159
4.4.4 管狀碳質/氧化鋁複合膜結合同步電混凝/電過濾程序去除水中新興污染物之綜合探討 168
4.5 管狀碳質/氧化鋁複合膜之薄膜積垢阻力探討 176
4.6 管狀碳質/氧化鋁複合膜結合同步電混凝/電過濾程序與其他處理程序之比較 182
第五章 結論與建議 187
5.1 結論 187
5.2 建議 190
參考文獻 191
附錄 215
博士在學期間發表之學術論文及發明專利 220

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