本研究的目的乃在於開發具有高通量及低逆溶質擴散量之碳複合薄膜，並應用於正滲透分離系統 (Forward osmosis, FO) 之中，期望能為全球水資源短缺問題做出貢獻。目前正滲透複合膜多以不織布或是高分子作為支撐膜材，本研究移除傳統支撐層材料，而以奈米碳管 (Carbon nanotubes, CNTs) 抽濾成薄膜作為支撐層，製備更薄且擁有更高水通表現之碳管薄膜。研究中透過聚多巴胺 (Polydopamine, PDA) 與聚乙烯醇 (Polyvinyl alcohol, PVA) 之協助，加強了CNT支撐層之親水性質與機械強度，接著使用傳統界面聚合法合成聚醯胺阻鹽層 (Polyamide, PA) ，完成薄膜的製備。研究內容包含表面形貌探討、表面官能基分析、親水性質、元素鍵結、粗糙度分析以及FO性能等測試。
研究結果顯示，PDA與PVA的聚合能使碳管更緊密黏著，加強薄膜在FO系統中之水流承受度，同時提升親水性質；不同抽濾含量可對薄膜厚度進行控制，厚度的降低能有效提升水通量；PVA濃度影響薄膜內部孔洞率，儘管濃度提升有助於機械性質的增加，卻會降低水通表現。本研究開發之碳管複合薄膜中，PVA0.25pCNT3-PA有最佳FO效能，在1M氯化鈉水溶液作為提取液與去離子水作為進流液的FO系統中，水通量為30.16 Lm-2h-1，逆溶質擴散量僅為9.34 gm-2h-1。此水通表現相較於較厚且未改質之碳複合薄膜高出近350%，再加上相對簡單的製程，說明了此研究在正滲透薄膜領域極具發展潛力。

This study aims to fabricate a thin-film composite (TFC) membrane with high water flux and low reverse solute flux in the application of forward osmosis (FO), hoping to make contribution to the global water crisis. Instead of using the traditional non-woven fabric or polymer material, carbon nanotube (CNT) is adopted as the substitutional support layer by the vacuum filtration method. Polydopamine (PDA) and polyvinyl alcohol (PVA) are used not only to increase the mechanical strength but also the hydrophilicity of the CNT membrane. Finally, a polyamide (PA) layer is fabricated by the interfacial polymerization method as the active layer. The characteristics of the membrane include surface morphology, surface functional groups, hydrophilicity, element bonding, surface roughness, and FO performance tests. Results show that PDA and PVA utilization sticks the CNT together, strengthening the tolerance of the membrane under FO testing system, meanwhile increasing the hydrophilicity. Membrane thickness can be controlled by using different CNT suspension filtration amount, and thinner membranes lead to higher water fluxes. The concentration of PVA influences the pores within the membrane and also plays an important role in the FO performance. The best FO properties are performed by PVA0.25pCNT3-PA, with a water flux of 30.16 Lm-2h-1 and reverse solute flux as low as 9.34 gm-2h-1. This water flux is almost 350% higher than that of the thicker CNT composite membrane. Therefore, the good FO performance and the relatively simple process of this study indicate great potential of this work in the application of FO field.

摘要----------------------------------------I
Abstract-----------------------------------II
致謝----------------------------------------III
目錄-----------------------------------------V
表目錄---------------------------------------X
圖目錄---------------------------------------XII
第一章 緒論----------------------------------1
1.1 前言--------------------------------------1
1.2 研究動機----------------------------------2
第二章 文獻回顧-------------------------------3
2.1 薄膜技術簡介-------------------------------3
2.1.1 薄膜技術發展-----------------------------3
2.1.2 薄膜種類---------------------------------4
(1) 對稱型薄膜、非對稱型薄膜--------------------5
(2) 微過濾、超過濾、奈米過濾、逆滲透薄膜----------5
(3) 有機薄膜、無機薄膜、有機/無機混合薄膜----------6
2.1.3 薄膜分離程序-------------------------------7
2.2 複合薄膜簡介與其製備----------------------------12
2.2.1 多孔支撐層之製備----------------------------12
(1) 拉伸法 (Stretching)----------------------------12
(2) 軌跡蝕刻 (Track etching)----------------------------13
(3) 電氣紡織 (Electrospinning)----------------------------13
(3) 相轉換法 (Phase inversion)----------------------------14
2.2.2 緻密選擇層之製備----------------------------14
(1) 界面聚合法------------------------------------------15
(2) 逐層堆疊法------------------------------------------16
2.3 正向滲透技術簡介---------------------------------------20
2.3.1 正向滲透技術發展與歷史-------------------------------20
2.3.2 正向滲透分離原理與應用----------------------------21
2.3.3 正向滲透技術之關鍵與瓶頸----------------------------22
(1) 濃度極化效應------------------------------------------23
(2) 逆溶質擴散------------------------------------------24
(3) 薄膜積垢------------------------------------------25
2.4 奈米碳管簡介------------------------------------------30
2.4.1 奈米碳管之結構與性質---------------------------------30
2.4.2 奈米碳管之製備方式------------------------------31
(1) 電弧放電法------------------------------------------32
(2) 雷射蒸發法------------------------------------------32
(3) 化學氣相沉積法------------------------------------------32
2.4.3 奈米碳管在水處理薄膜領域之應用----------------------------33
2.5 本實驗室水處理主題研究回顧---------------------------------39
第三章 實驗方法與分析------------------------------------------42
3.1 實驗用化學藥品、設備與分析儀器----------------------------42
3.1.1 超音波震盪機------------------------------------------43
3.1.2 電磁加熱攪拌機------------------------------------------43
3.1.3 場發射掃描式電子顯微鏡-----------------------------------43
3.1.4 穿透式電子顯微鏡------------------------------------------44
3.1.5 拉曼光譜儀------------------------------------------44
3.1.6 傅立葉轉換紅外光譜儀-------------------------------------45
3.1.7 X射線光電子能譜儀------------------------------------------45
3.1.8 水接觸角量測儀------------------------------------------46
3.1.9 原子力顯微鏡------------------------------------------47
3.1.10 正滲透效能測試裝置-------------------------------------47
3.2 實驗方法與步驟------------------------------------------55
3.2.1 支撐層製備---------------------------------------------55
(1) TCNT/PVA支撐層------------------------------------------55
(2) pCNT/PVA支撐層------------------------------------------56
(3) PVApCNT支撐層------------------------------------------57
3.2.2 聚醯胺阻鹽層製備------------------------------------------57
第四章 結果與討論------------------------------------------62
4.1 以奈米碳管作為支撐層之可行性探討----------------------------62
4.2 TCNT/PVA、pCNT/PVA、PVApCNT支撐層之分析與比較--------------63
4.2.1 SEM形貌分析------------------------------------------63
4.2.1.1 表面形貌------------------------------------------63
4.2.1.2 截面形貌------------------------------------------64
4.2.2 TEM分析------------------------------------------65
4.2.3 拉曼光譜分析------------------------------------------65
4.2.4 FTIR光譜分析------------------------------------------66
4.2.5 水接觸角分析------------------------------------------66
4.2.6 XPS元素分析------------------------------------------67
4.2.7 AFM表面粗糙度分析---------------------------------------68
4.3 聚醯胺阻鹽層之分析------------------------------------------81
4.3.1 SEM形貌分析------------------------------------------81
4.3.2 FTIR光譜分析------------------------------------------81
4.3.3 AFM表面粗糙度分析------------------------------------------82
4.4 CNT碳複合膜正向滲透效能探討----------------------------85
4.4.1 溫度對於FO效能之影響---------------------------------------85
4.4.2 不同CNT支撐層對FO效能之影響與比較----------------------------85
4.4.3 提取液濃度與FO、PRO模式對於效能之影響--------------88
4.4.4 A、B、S數值------------------------------------------89
4.4.5 本研究製備之正滲透薄膜與商用及其他研究成果之效能比較---------89
4.4.6 有機溶液濃縮測試------------------------------------------90
第五章 結論--------------------------------------------------98
第六章 參考文獻------------------------------------------100

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