臺灣博碩士論文加值系統

近年來正滲透（Forward osmosis，FO）薄膜技術逐漸成熟，以半透膜區隔進流溶液（Feed solution，FS）與高濃度溶質的驅動溶液（Draw solution，DS），透過天然的濃度梯度產生滲透壓差，可在驅動溶液中獲取高品質的濾液。為了克服目前薄膜所面臨的主要問題：濾液水通量低與反向溶質擴散現象，本研究旨在於優化複合式正滲透薄膜（Thin film composite FO membrane，TFC-FO）的製備條件，先針對表面聚醯胺（Polyamide，PA）活性層的製備進行優化，分別添加沸石咪唑酯骨架（ZIF-8）奈米顆粒於在間苯二胺（m-Phenylenediamine, MPD）及均苯三甲醯氯（Trimesoyl chloride, TMC）溶液中以提升薄膜的分離成效。並針對聚碸（Polysulfone，PSf）支撐層進行田口實驗設計及其他改質方式，以找出最佳的製備條件；後續分別在去離子水(DI)、積垢合成水、養殖廢水中個人與醫療保健用品（Pharmaceuticals personal care products，PPCPs）的去除與回收，以評估製備薄膜之操作效益。
研究結果顯示，PSf薄膜的良好製備參數為2.0mmole的硝酸鋅及16mmole的2-甲基咪唑，PA層則為0.025%的ZIF-8顆粒在TMC溶液中。將0.025%的ZIF-8顆粒加進在TMC溶液中(命名為PA0.025)具有良好的薄膜選擇性（62.9 L/ mole）與最佳的結構參數（152μm）。而將2.0mmole的硝酸鋅及16mmole的2-甲基咪唑加進PSf塗佈液中（製成的薄膜命名為PSf2.0-PA），具有最佳的PPCPs去除率，在積垢合成水中，對已解離的PPCPs（IBU(ibuprofen)、SMX (sulfamethoxazole)、DIA (sulfadiazine)）因靜電相斥作用，去除率均可高達97.0%以上，而對極高疏水性的Triclosan，通過反萃取實驗證實會其會吸附於薄膜表面而逐漸溶解貫穿導致去除率降低，對以分子態存在於水體當中的中性Carbamazepine，主要以篩分為去除機制，去除率也可高達97.9%。養殖廢水的回收實驗方面，PA0.025膜具有良好的親水性及抗垢性，在實驗初期表現出最高的水通量（8.05 L/m2 h），長時間測試下的最終累積產水量為425.1 L/m2。

Forward osmosis (FO) technology has been gradually developed and applied, which uses a semi-permeable membrane to separate the feed solution (FS) and the draw solution (DS) with high concentration of solutes to provide the driving force of concentration gradient. However, the major challenges of applying FO technology are low permeate flux and the occurrence of reverse solute flux. Therefore, we evaluated the key parameters of synthesizing the polysulfone (PSf) support layer and polyamide (PA), respectively, to optimize the performance of thin-film composite FO membranes (TFC-FO). Firstly, the preparation of surface polyamide (PA) active layer was optimized, and zeolite imidazolate framework (ZIF-8) nanoparticles were added to m-Phenylenediamine (MPD) and trimesyldiamine respectively. Taguchi experimental design and other modification methods for the polysulfone (PSf) support layer were carried out to find the best preparation conditions; the subsequent experiments were carried out in deionized water (DI), synthetic fouling water, and aquaculture wastewater. and the removal and recycling of pharmaceuticals personal care products (PPCPs included carbamazapine (CBZ), triclosan (TRI), ibuprofen (IBU), sulfadiazine (DIA), sulfamethoxazole (SMX) and sulfamethazine (SMZ)) to evaluate the operational benefits of preparied membrane.
The results show that the good preparation parameters of PSf membrane are 2.0 mmole of zinc nitrate and 16 mmole of 2-methylimidazole, and the PA layer is 0.025% ZIF-8 particles in TMC solution. The addition of 0.025% ZIF-8 particles in TMC solution (named PA0.025) has good membrane selectivity (62.9 L/mole) and the best structural parameters (152 μm). However, adding 2.0 mmole of zinc nitrate(ZnNO3)2· 6H20 and 16 mmole of 2-methylimidazole to the PSf coating solution (the prepared film was named PSf2.0-PA) had the best removal rate of PPCPs, and in the fouling synthetic water, The rejection of dissociated IBU, SMX, and DIA can achieve 97.0due to electrostatic repulsion. The extremely hydrophobic TRI, it was confirmed by back-extraction experiments. It will be adsorbed on the surface of the membrane and gradually dissolved and penetrated, resulting in a decrease in the removal rate. and low rejection of highly hydrophobic tricolson because of adsorption and penetration through membranes.
For the neutral CBZ that exists in the water body in the molecular state, the removal mechanism is mainly based on sieving, and the rejection can also be as high as 97.9%. In the recycling experiment of aquaculture wastewater, the PA0.025 membrane has good hydrophilicity and scale resistance, showing the highest water flux (8.05 L/m2h) at the beginning of the experiment, and the final cumulative water production under long-term testing is 425.1 L/m2.

摘要 I
Abstract II
致謝 IV
圖目錄 VIII
表目錄 XI
第一章 緒論 2
1.1研究緣起 2
1.2研究目的 3
第二章 文獻回顧 4
2.1正滲透的原理及應用 4
2.1.1 正滲透的原理及特性 4
2.1.2 正滲透的操作方式 6
2.1.3 正滲透的技術應用 7
2.2影響正滲透操作的關鍵因子 10
2.2.1 薄膜特性 11
2.2.2 驅動溶液 13
2.2.3 濃度極化 15
2.2.4 水質特性 17
2.3金屬有機骨架材料特性 19
2.3.1 MOF材料簡介 19
2.3.2金屬有機骨架的合成方法 20
2.4正滲透膜製備技術 20
2.4.1 相轉換 21
2.4.2 界面聚合 25
2.4.3 奈米複合式薄膜 26
2.5正滲透膜分離機制與模式 28
2.5.1分離機制 28
2.5.2質傳係數與滲透壓計算 30
2.5.3滲透傳輸預測公式 32
第三章 研究方法及步驟 37
3.1研究方法 37
3.2實驗材料 38
3.2.1 TFC-FO 製膜材料 38
3.2.2改質材料 39
3.2.3 污染物篩選 41
1. 醫療與個人保健用品（PPCPs） 41
3.3製備ZIF-8顆粒 46
3.4製膜程序與實驗設計 46
3.4.1 PSf支撐層製備 46
3.4.2 PA活性層製備 48
3.5薄膜操作效能與分離成效評估 49
3.5.1 FO模組及操作參數 49
3.5.2 水通量、反向溶直通量及反向溶質通量選擇性計算 51
3.5.3 PPCPs去除率及膜面吸附量 52
3.5.4 實廠廢水效能評估指標 53
3.6薄膜特性分析與結構參數計算 53
3.6.1 薄膜特性分析 53
3.6.2 結構參數計算 55
第四章 結果與討論 58
4.1正滲透薄膜改質(PA活性層) 58
4.1.1 添加不同劑量之ZIF-8改質FO表層膜 58
4.1.2正滲透薄膜改質(PA活性層)小結 66
4.2正滲透薄膜改質(PSf支撐層) 67
4.2.1硝酸鋅及2-甲基咪唑改質PSf支撐層 67
4.2.2光接枝改質PSf支撐層 72
4.2.3正滲透薄膜改質(PSf支撐層)小結 76
4.3正滲透薄膜改質(PSf支撐層、PA活性層共同改質) 78
4.3.1 ZIF-8共同改質PSf支撐層、PA活性層和光接枝改質/ZIF-8混合膜 78
4.3.2正滲透薄膜改質(PSf支撐層、PA活性層共同改質)小結 81
4.4結構參數與薄膜選擇性 82
4.4.1 結構參數與薄膜選擇性評估薄膜優異性 82
4.4.2 結構參數與薄膜選擇性小結 83
4.5 PPCPs去除實驗 84
4.5.1 製備薄膜在DI水中對PPCPs的去除成效 84
4.5.2製備薄膜在合成積垢水中對PPCPs的去除成效 86
4.5.3製備薄膜在養殖廢水中對PPCPs的去除成效 90
4.5.4 PPCPs去除實驗小結 96
第五章 結論與建議 97
5.1結論 97
5.2建議 98
參考文獻 99

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