臺灣博碩士論文加值系統

近年，各國為了因應水源及能源匱乏的現況，爰開發綠色節能的水處理技術並回收珍貴的水資源，已成為全球關注的議題。本研究採用低耗能的正滲透（Forward osmosis, FO）技術，其透過進流溶液（Feed solution, FS）與驅動溶液（Draw solution, DS）間自然產生的滲透壓差，驅使水分子從FS通過半透膜移動至DS，可達到水回收並分離濃縮FS中的污染物，但FO在操作過程需克服低濾液通量及反向溶質擴散等挑戰。對此，本研究利用栗子殼（Castanea shell, CS）及木質素（Lignin, LG）二種不同木質纖維素廢棄物，透過水萃法改質複合式正滲透薄膜（Thin film composite FO, TFC-FO）的表面活性層（Polyamide, PA），及直接添加法改質TFC-FO的底部支撐層（Polysulfone, PSf），並測試在不同木質纖維素的添加方式、粒徑、及濃度等因子，期能大幅提升膜面親水性及水通量，並降低反向溶質通量。後續，將改質前後的TFC-FO應用於六種在台灣環境水體中常被偵測到的醫藥與個人保健用品（Pharmaceuticals personal care products, PPCPs），以確認對環境中新興微量有機物的去除成效，並進一步應用于海淡鹵水的分離以回收珍貴水資源，同時濃縮鹵水中的貴重金屬供後續再利用。
研究結果發現，直接添加1 wt%的LG（粒徑為38~53 μm）改質PSf層（命名為LG-S1），具有良好的水通量及穩定的反向溶質通量（31.3 LMH、3.81 nMH）。此外，水萃添加1 wt%的CS改質PA層（命為CS-AW1）及直接添加0.5 wt%的CS（粒徑為25~38 μm）改質PSf層（命為CS-S0.5），均具有最佳之水通量及反向溶質通量（9.2、8.6 LMH與0.08、0.67 nMH）且CS-AW1改質膜具有最佳的結構參數（75 μm）。各薄膜除了對於疏水性極高的Triclosan僅有18%–30%的去除率，對其餘PPCPs的去除率均可達到80–100%，然而因添加CS從而使Ibuprofen與其產生氫鍵鍵結使吸附量上升。對於海淡鹵水的回收應用，發現CS-AW1改質膜在模擬鹵水下，連續操作24 h的水回收率及各金屬濃縮倍數可達到50%及1-2倍，並將其應用於實廠海淡鹵水下，實驗初期的水通量明顯優於未改質膜，而經由長時間測試下，其具有良好的水回收率（45%），且對於Na+與Mg2+的濃縮倍數可達1-2倍，提升後續再利用的可行性。

To deal with the global isusue of water and energy scarcity, it is urgent to develop green and energy-saving water treatment technologies as well as recycle precious water resources. Forward osmosis (FO) is a low-energy water separation technology that drives water molecules through the semi-permeable membrane using the naturally occurred osmotic pressure difference between the feed solution (FS) and the draw solution (DS) to achieve water recovery and the separation/concentration of pollutants in FS. However, there remains several challenges that need to be overcome for practically application, such as low permeate flux and the loss of DS solute due to its reverse diffusion during operation. In this study, we used two different lignocellulosic biowastes, Castanea shell (CS) and lignin (LG), to modify the polyamide (PA) and polysulfone (PSf) layers of the thin-film composite (TFC) FO membranes (TFC-FO). Experimental factors including different addition methods (water extraction or direct addition), particle sizes, and dosages, were systematically evaluated. The prepared membranes were used for the removal of six pharmaceutical and personal care products (PPCPs) that are commonly detected in the aqatic envurinment in Taiwan, as well as for brine recovery from sea water desalination.
Results showed that the direct addition of 1 wt% LG (with a particle size of 38-53 μm) to modify the PSf layer (referred to as LG-S1) resulted in improved water flux and stable reverse solute flux (31.3 LMH and 3.81 nMH). Furthermore, water extraction with the addition of 1 wt% CS to modify the PA layer (referred to as CS-AW1) and direct addition of 0.5 wt% CS (with a particle size of 25-38 μm) to modify the PSf layer (referred to as CS-S0.5) exhibited optimal water flux and reverse solute flux (9.2 and 8.6 LMH, and 0.08 and 0.67 nMH, respectively). CS-AW1 modified membrane demonstrated the best structural parameters (75 μm).All membranes achieved removal rates of 80-100% for most PPCPs, except for Triclosan, which showed only 18-30% removal due to its high hydrophobicity. However, the addition of CS increased the adsorption of Ibuprofen due to the formation of hydrogen bonding.For the recovery and reuse of seawater desalination brine, CS-AW1 modified membrane exhibited a water recovery rate of 50% and metal concentration factors of 1-2 when tested under simulated brine conditions for continuous operation of 24 hours. The membrane was also applied to actual seawater brine in a pilot plant, showing superior initial water flux compared to the unmodified membrane. Over extended testing periods, it demonstrated a good water recovery rate of 45% and a concentration factor of 1-2 for Na+ and Mg2+, enhancing the potential for subsequent reuse.

摘要 I
Abstract II
致謝 III
目錄 IV
圖目錄 VII
表目錄 IX
第一章 緒論 1
1.1研究緣起 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正滲透原理及特性 3
2.1.2正滲透的操作方式 4
2.1.3正滲透的技術應用 4
2.2影響正滲透操作成效的關鍵因子 7
2.2.1薄膜特性 9
2.2.2驅動溶液組成 9
2.2.3濃度極化 11
2.2.4水質特性 12
2.3木質纖維素材料特性 13
2.4正滲透薄膜製備技術 15
2.4.1相轉換 15
2.4.2界面聚合（Interfacial polymerization, IP） 16
2.4.3奈米複合式薄膜（Thin film nanocomposite, TFN） 17
2.5正滲透膜的分離機制與模式 17
2.5.1薄膜的分離機制 17
2.5.2質傳係數與滲透壓計算 19
2.5.3滲透傳輸預測公式 20
第三章 研究方法及步驟 21
3.1研究方法 21
3.2實驗材料 22
3.2.1 TFC-FO製備材料 22
3.2.2改質材料 23
3.2.3污染物篩選 23
3.3實驗步驟與設計 25
3.3.1 PSf支撐層製備 25
3.3.2 水萃溶液製備 27
3.3.3 PA活性層製備 28
3.4薄膜操作效能與分離成效分析 29
3.4.1 FO模組及操作參數 29
3.4.2水通量、反向溶質通量與薄膜選擇性計算 30
3.4.3結構參數計算 31
3.4.4 PPCPs去除率及膜面吸附量 32
3.4.5鹵水回收之效能評估 34
3.4.6薄膜與材料特性分析 35
第四章 結果與討論 40
4.1生質物特性分析 40
4.1.1特性組成鑑定 40
4.1.2小結 44
4.2以木質素改質正滲透薄膜 45
4.2.1 水萃LG改質PA層 45
4.2.2直接添加LG改質PSf層 48
4.2.3小結 52
4.3以栗子殼改質正滲透薄膜 54
4.3.1 水萃CS改質PA層 54
4.3.2直接添加CS改質PSf層 56
4.3.3 CS雙層改質 62
4.3.4小結 66
4.4正滲透薄膜對PPCPs的分離成效評估及結構參數 67
4.4.1 PPCPs的去除成效 67
4.4.2結構參數 68
4.4.3小結 70
4.5正滲透薄膜對鹵水的分離成效評估 71
4.5.1模擬鹵水的濃縮成效 71
4.5.2海淡鹵水的濃縮成效 75
4.5.3小結 79
第五章 結論與建議 80
5.1結論 80
5.2建議 81
參考文獻 82

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