正滲透(FO)屬於新興的薄膜分離技術，其利用濃度差而非壓力差作為過濾的驅動力，故可在獲得高品質濾液的同時，大幅降低能量的消耗並延緩膜面積垢的產生。目前商業化的正滲透薄膜相當少，仍處於研發階段，更無法以現有逆滲透(RO)薄膜作為使用，因此開發功能性的正滲透薄膜是有其必要性。本研究以聚碸(Polysulfone,PSF)為聚合單體，透過相轉換法製備多孔聚碸PSf支撐層，而後利用界面聚合法形成聚醯胺(Polyamide, PA)選擇層，以製備複合薄膜(thin-film composite membrane, TFC)。研究分別使用氧化石墨烯(Graphene Oxide, GO)改質PA選擇層、親水性奈米顆粒（Nanoparticles, NPs）改質PSf支撐層、及利用共鑄法優化支撐層，以期利用材料本身的親水性及結構優化提升薄膜的通量表現及分離效能；研究透過薄膜物化特性鑑定、結構參數計算與量化、及染劑去除測試，以選定最佳的薄膜改質配方，並將最佳改質膜與原膜應用於實廠污泥濃縮並回收水的測試，以評估其實廠應用性。
研究結果發現，以相轉換製備TFC膜，得知製備溫度(70℃)及適當的塗佈高度(225 µm)，並避免水氣摻雜於溶液中，可獲得較高品質的PSf支撐層。針對PA選擇層的製備條件，則選擇使用等量的MPD與TMC溶液，在20 mL的添加量下可以獲得較高通量的表現；界面聚合應選擇PSf支撐層頂部進行反應，由於頂部膜面平滑，有利於PA選擇層生成。以此法所製備出的原始膜具有8.7 LMH的水通量及0.86 nMH的反向溶質通量。
透過添加商業化GO改質PA選擇層，能進一步改善通量表現，在最佳添加濃度0.0175 wt％時，可製備出具有最高水通量(14.0 LMH)及最低的反向溶質通量(0.29 nMH)的FO薄膜。隨著GO濃度添加，能夠增加親水滲透性及孔隙率，但在較高GO添加濃度(> 0.02 wt%)時，會導致GO團聚，故降低通量表現及孔隙率 。在以奈米顆粒改質PSf支撐層的部份，對通量表現沒有改善，且添加高度親水性材料於疏水性的PSf聚合溶液可能導致結合性差，進而導致PA選擇層的缺陷。以共鑄法改質PSf支撐層，薄膜的通量表現並沒有得到改善，透過添加GO改質PA選擇層效果也不彰，表示共鑄法可能改變膜面形貌，進而影響GO改質效果。所製備的薄膜均進一步進行結構參數的量測與量化，計算發現GO改質PA層在添加濃度為-0.0175%具有最高的反向溶質通量選擇性(0.83 L/g)，其S值(274 µm) 與最低結構參數(259 µm)相近，此條件視為最佳製備條件。
在染劑去除測試部分，GO改質PA選擇層是具有較穩定的去除效率(96%-99.4%)，另外，在實廠活性污泥測試部分，有賴於GO改善初始水通量，延緩積垢情形的產生，隨著時間遞增，最佳改質膜與原始膜濃縮係數得到類似的趨勢。運行24小時的水回收率達到40.02%，原始膜則為31.15%。此積垢情形經過DI水連續沖洗，僅有部分積垢層被沖洗下來，判斷GO對於抗垢程度的優化仍需要改善。
重複性及再現性實驗中，使用改良後界面聚合法製備TFC膜，得知相轉換所需水量0.5 (L/cm3)將得到較好品質PSf支撐層，使用TMC濃度0.15 (w/v%)，並用水沖洗成膜以及固化溫度調整為80℃，將可以得到最佳品質TFC膜，獲得最高通量9.7 LMH及0.7 nMH的通量表現。

Forward osmosis (FO) is an emerging membrane separation technology, which is driven by the osmotic pressure difference across a semipermeable membrane rather than hydraulic pressure as a driving force. In addition, Through FO can obtain a high-quality permeate reduce energy consumption and prevent fouling. However, a small number of commercial forward osmosis membranes are available in the market, and FO membranes are not replaceable usiing reverse osmosis (RO) membranes because of the different design purposes. Therefore, it is essential to develop functional forward osmosis membranes. In this study, polysulfone (PSf) was used fabricate the porous support layer of FO membranes by phase inversion method, and then polyamide active (PA) layer was formed on PSf substrate by interfacial polymerization to fabricate the thin-film composite (TFC) FO membranes. The FO membranes were further modified by adding Graphene oxide (GO) in PA active layer, and hydrophilic nanoparticles (NPs) in PSf substrate with the expectation to improve the permeate flux (Jw), selectivity 〔Jw / reversesolute flux (Js)〕, and anti-fouling property of the FO membranes. Moreover, the co-casting method for PSf substrate was also tested to optimize the PSf support layer. The virgin and modified membranes evaluated in terms of permeate flux, intrinsic transport parameters, physicochemical characterization, and dye rejection to determine the optimize membrane modification receipe. Finally, The virgin and the best-modified membranes were applied to concentrate the waste activated sludge for water recovery as valuable resource.
The results of the study indicated that several key parameters need to be carefully controlled during the fabricated of PSf substrate by phase inverse method, inducing
thoroughly degassing, sealing, and temperature control at 70℃ with the optimal casting height of 225 μm. As for the fabrication of the active layer, the equal amount (20mL:20mL) of m-Phenylenediamine (MPD) and 1,3,5-Benzenetricarboxylic acid chloride (TMC) monomers on the top side of PSf substrate to can achieve interfacial polymerization with better membrane seperation performance. (Jw = 8.7 LMH , Js = 0.86 nMH)
Adding GO to modify PA active layer can improve FO separation efficiency with the highest Jw of 14.0 LMH and the lowest Js of 0.29 nMH at the optimal GO dosage of 0.0175 wt%. The water permeability and membrane porosity increased with increasing GO dosage; however GO agglomeration may occur at dosage (>0.02%), which deteriorate Jw and increase Js. On the other hand, the temptation of adding by hydrophilic Nanoparticles (NPs) to modify PSf substrate did not pay back, which may result from the poor bonding, between the highly hydrophobic PSf and the hydrophilic NPs, leading to defects on the further formed PA active layer. The co-casting of polyetherimide (PEI) modify to PSf substrate the previous developed base did not reward as well, The PA layer modified with dosage of GO did not exhibit any improve in membrane performance, indicating that the co-casting method affected the morphology and/or even the structure of PSf substrate so as to the PA layer despite the dosage of GO for PA modification. After evaluating the structural factor, the FO membrane with PA layer modified using 0.0175wt% GO exhibited the lowest S value of 259μm with the highest selectivity of 0.83 L/g, and this was regarded as the best modification recipre for FO membranes. For dye removal tests, the GO modified membranes exhibited relatively stable removal efficiency for all selected dyes compared to thevirgin membranes (96%-99.4%). In addition, the virgin and GO modified membranes were further applied for activated sludge thickening. The GO modified membrane exhibited considerably higher initial permeate flux than the virgin membrane; however, the decrease of permeate flux with increasing time for both membranes. The total water recovery reached 40.02% and 31.15% for the modified and virgin membranes, respectively. Only part of the foulant can be washed out using DI flushing and the anti-fouling of the fabricated membranes can be further improved.
Finally, the procedures of the interfacial polymerization method were further evaluated to test the performance and stability of the FO membranes. It was found that the water volume of 0.5 L/cm3 to form PSf substrate by phase inversion can result in a good PSf substrate with fingershape structures to facilitate water transport. In the meantime, the procedures for PA layer formation were also evaluated. The results indicated that TMC concentration 0.15 w/v% for interfacial polymerization followed by DI washing of membrane surface then curing at 80℃ in the oven for 5 min can further stabilize the FO membrane with higher performance of 9.7 LMH and 0.7 nMH.

摘要
Abstract
致謝
目錄
圖目錄
表目錄
第一章 緒論
1.1 研究緣起
1.2 研究目的
第二章 文獻回顧
2.1 正滲透的原理與應用
2.1.1 正滲透原理與特性
2.1.2 正滲透的操作方式
2.1.3正滲透技術應用
2.2 影響正滲透操作成效關鍵因子
2.2.1 薄膜特性
2.2.2 驅動溶液
2.2.3 水質特性
2.2.4 濃度極化
2.3 正滲透製備技術
2.3.1相轉換
2.3.2界面聚合
2.3.3其他
2.4 正滲透分離機制與模式
2.4.1 分離機制
2.4.2 質傳係數跟滲透壓計算
2.4.3 效能預測模式
第三章 研究方法及步驟
3.1 研究方法
3.2 實驗材料與設備
3.2.1 PSf支撐層材料
3.2.2 表層PA選擇層材料
3.2.3 PSf支撐層改質材料
3.2.4 PEI-PSf共鑄膜材料
3.2.5 染劑篩選
3.2.6 正滲透過濾系統
3.3 實驗設計與步驟
3.3.1 PSf支撐層製備
3.3.2 界面聚合法製備PA表層
3.3.3 PEI-PSf共鑄支撐層製備
3.3.4 改良界面聚合法製備PA表層
3.4 薄膜操作效能測試與特性參數量測
3.4.1 水通量、反向溶質通量及反向溶質通量選擇性計算
3.4.2 水滲透係數計算(FO法v.s.RO法)
3.4.3 結構參數計算
3.4.4 薄膜染劑去除實驗
3.5 分析方法
3.5.1 膜面親疏水性分析
3.5.2 薄膜厚度分析
3.5.3 染劑濃度分析(UV)
3.5.4 膜面形貌分析
3.5.5 薄膜孔隙率測量
3.5.6 實廠廢水效能評估指標
4.1 正滲透薄膜各層製備條件確認
4.1.1 TFC薄膜製備條件確認
4.1.1.1 PSf支撐層製備條件確認
4.1.1.2 PA選擇層製備條件確認
4.1.1.3 水合處理(Hydration)
4.1.2 改良界面聚合法製備TFC薄膜因子確認
4.1.2.1 PSf支撐層製備條件確認
4.1.2.2 PA選擇層製備條件確認
4.1.3 正滲透薄膜各層製備條件確認之小結
4.2正滲透薄膜改質
4.2.1 PA選擇層改質
4.2.2 PSf支撐層改質
4.2.3 PSf支撐層共鑄
4.2.4正滲透薄膜改質小結
4.3 結構參數與反向溶質通量選擇性
4.3.1 FO法求取結構參數的合理性
4.3.2 使用結構參數與反向溶質通量選擇性評估TFC膜效能
4.3.3 結構參數與反向溶質通量選擇性之小結
4.4 染劑去除效率測試
4.4.1 GO改質PA選擇層之染劑去除效率
4.4.2 奈米顆粒改質PSf支撐層之染劑去除效率
4.4.3 共鑄支撐層之染劑去除效率
4.4.4 染劑去除效率測試小結
4.5 分離機制確認
4.5.1 染劑分離機制評估
4.5.2 分離機制確認之小結
4.6 實廠廢水處理成效評估
4.6.1 實廠廢水處理成效
4.6.2 實廠廢水處理成效之小結
第五章 結論與建議
5.1 結論
5.2 建議
參考文獻
附錄一 導電度檢量線

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