臺灣博碩士論文加值系統

本研究採用能耗極低的正滲透（Forward osmosis, FO）技術，期透過不同方式優化複合式（Thin film composite, TFC）正滲透薄膜（TFC-FO）的分離成效及產水率。首先，透過負壓保存縮短TFC-FO薄膜的調理時間。使用硝酸鐵九水合物中的Fe3+嫁接檸檬酸鈉中的羧基（-COOH）改質薄膜的頂部聚醯胺（Polyamide, PA）活性層（Active layer, AL）以優化薄膜的親水性，進而提升水通量（Water permeate flux, JP），並透過金屬有機骨架（Material organic framework, MOF）的沸石唑酯骨架（Zeolitic imidazolate framework 67, ZIF-67）的結晶顆粒及其合成材料硝酸鈷六水合物（Cobalt（II）nitrate hexahydrate, CNH）和2-甲基咪唑（2-Methyl-1H-imidazole, 2-Hmim）改質TFC-FO的聚碸（Polysulfone, PSf）支撐層（Support layer, SL）以及PA活性層 。接續，將上述分層改質PA/PSf層的最適參數進行雙層改質。測試改質前後薄膜對六種台灣常見的醫藥與個人保健用品（Pharmaceuticals personal care products, PPCPs）之去除成效及濃縮實廠染機廢水回收，並將整個流程進行生命週期評估 （Life cycle assessment, LCA），以量化其環境衝擊影響的效益。
研究結果顯示，在負壓條件下成功將薄膜調理時間縮短為原製程的11%，且保有與未改質原膜（Virgin）相同的分離效能。使用Fe3+嫁接-COOH之後讓水通量上升為Virgin的140%。以ZIF-67顆粒或合成材料CNH和2-Hmim改質PA和PSf的通量測試結果顯示，以0.025wt%的ZIF-67顆粒改質活性層之後，水通量上升為Virgin的153%。而在PSf改質中的最佳組是以25mM之CNH和2-Hmim（ZSS25）改質後的薄膜，水通量上升為Virgin的156%。改質膜中除了同時對PA和PSf改質的膜以外其餘在PPCPs分離成效測試中的效能有所提升。此外，實廠染機廢水回用的結果發現，ZSS25成功將染機廢水回收耗時減半，同時也將染色強度提升為原來的一倍。故本研究製備的ZSS25改質膜具最佳的水通量、及分離成效，將有助於提供實廠染整廢水回收再利用。本研究中成功以負壓保存的方式提升了薄膜製程的效率，並以ZIF-67顆粒以外的形式（合成材料）改質PSf，染機廢水回用的部分，雖在提濃後染色強度未達到原液的100%，但確實成功提升其染色強度，未來可將其作為再生染液，提供給市場更多的選擇。

關鍵字：複合式正滲透薄膜改質（TFC-FO）、金屬有機骨架（MOF）、染整廢水回收、生命週期評估（LCA）

This study employed energy-efficient forward osmosis (FO) technology to optimize the separation efficiency and water productivity of thin-film composite forward osmosis membranes (TFC-FO) through various means. Firstly, the conditioning time of TFC-FO membranes was shortened by negative pressure preservation. The top polyamide (PA)active layer was modified with carboxyl groups (-COOH) grafted from sodium citrate in iron nitrate nonahydrate (Fe3+) to enhance the hydrophilicity of the membrane, thereby improving water permeate flux (JP). The polyimide (Polysulfone, PSf) support layer of TFC-FO was modified using crystalline particles of zeolitic imidazolate framework 67 (ZIF-67) and synthesized material cobalt (II) nitrate hexahydrate (CNH) and 2-methyl-1H-imidazole (2-Hmim). Furthermore, the optimal parameters of the modified PA/PSf layer were used for dual-layer modification. The membranes before and after modification were tested for their response to six commonly found pharmaceuticals and personal care products (PPCPs) in Taiwan, as well as concentrated wastewater from dyeing machines, followed by dyeing experiments. A life cycle assessment (LCA) was conducted for the entire process. The research results showed that under negative pressure conditions, the membrane conditioning time was reduced to 11% of the original process while maintaining the same efficiency as the virgin membrane. The water flux increased by 140% after grafting -COOH. The flux testing results for PA modification using ZIF-67 particles or synthesized material showed a 153% increase in water flux after modification with 0.025wt% ZIF-67 particles in the active layer. The best PSf modification was achieved using 25mM CNH and 2-Hmim (ZSS25), resulting in a 156% increase in water flux. Apart from the membranes modified simultaneously for PA and PSf, the performance of other modified membranes showed improvement in PPCPs separation efficiency testing. In addition, the results of reusing wastewater from dyeing machines indicated that ZSS25 reduced the recycling time by half and doubled the dyeing intensity. Therefore, the ZSS25-modified membrane prepared in this study exhibited optimal water flux and separation efficiency, contributing to the recycling and reuse of wastewater from dyeing plants. The study successfully improved the efficiency of membrane fabrication through negative pressure preservation and modified PSf using forms other than ZIF-67 particles (synthesized material). Although the dyeing intensity after concentration did not reach 100% of the original liquid, it was indeed increased, making it a potential candidate for regenerated dye solutions, providing customers with more options.

Keyword：Thin film composite (TFC); Forward osmosis (FO); Modification; Metal organic framework (MOFs); Pharmaceuticals and personal care products (PPCPs); Recycling of Textile Wastewater

摘要 I
致謝 V
第一章、緒論 1
1.1 研究起源 1
1.2研究目的 2
第二章、文獻回顧 3
2.1正滲透的原理及應用 3
2.1.1滲透模式的種類及原理 3
2.1.2正滲透操作模式與特性 4
2.1.3正滲透技術的應用 5
2.2影響正滲透分離成效的關鍵因子 6
2.2.1薄膜特性 7
2.2.2薄膜活性層功能及面向 8
2.2.3濃度極化（Concentration polarization, CP） 8
2.2.4 進料溶液特性及選擇 10
2.2.5提取液特性及選擇 11
2.3薄膜改質材料之種類與特性 12
2.3.1 奈米顆粒（Nano particles, NPs） 13
2.3.2有機金屬骨架材料（Metal organic framework, MOF） 13
2.3.3 親水性官能基和其螯合劑 16
2.4複合式薄膜的製備與改質技術 17
2.4.1支撐層製備方法 18
2.4.2活性層製備方法 21
2.4.3複合式薄膜 21
2.4.4複合式薄膜改質技術 22
2.5薄膜分離機制與模式 24
2.5.1 薄膜分離機制 24
2.5.2質傳係數與滲透壓計算 25
2.5.3.滲透傳輸運算公式 26
2.6生命週期影響評估 27
2.6.1 LCA規劃流程 28
第三章、研究方法 29
3.1研究架構 29
3.2實驗藥品及材料 30
3.2.1原膜與改質材料 30
3.2.2污染物篩選與提取溶液選用 32
3.3薄膜製備與實驗設計 35
3.3.1 PSf支撐層製作與改質 36
3.3.2PA活性層製作與改質 37
3.3.3 薄膜負壓保存調理 39
3.4 薄膜效能測試與特性分析 40
3.4.1薄膜水、反向鹽質通量測試及選擇性 40
3.4.2 水、鹽滲透係數 41
3.4.3 結構參數 42
3.4.4能源消耗 42
3.4.5 PPCPs去除率及膜面吸附量 43
3.4.5 薄膜特性分析 45
3.4.6 染劑濃度分析（UV） 47
3.4.7 實廠廢水效能評估指標 47
3.5生命週期影響評估 48
第四章、結果與討論 50
4.1負壓條件優化與嫁接親水基改質 50
4.1.1負壓條件測試 50
4.1.2嫁接Fe3+親水基改質PA層 52
4.1.3 小結 54
4.2 ZIF-67分層改質TFC-FO薄膜 55
4.2.1 直接添加ZIF-67改質PA層 55
4.2.2 合成生成ZIF-67改質PA層 58
4.2.3 直接添加ZIF-67改質PSf層 60
4.2.4合成生成ZIF-67改質PSf層 62
4.2.5 結構參數 65
4.2.6小結 66
4.3 PPCPs及染料的去除成效測試 67
4.3.1 PPCPs的去除成效 67
4.3.2染料的去除成效 69
4.3.3小結 71
4.4實廠廢水回收與再利用 72
4.5膜分離程序生命週期影響評估 84
4.5.1 盤查系統邊界與條件假設 84
4.5.2 盤查清單建立與分析方法選用 84
4.5.3環境影響評估分析結果 85
4.5.4小結 91
第五章 結論與建議 92
5.1結論 92
5.2建議 93
參考文獻 94

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