本研究構想利用摻合法製備金屬-有機框架(Metal-organic framework，MOF)/polysulfone複合膜，於鑄膜液中將有機連接劑(organic linker)及金屬離子溶解於鑄膜溶液以濕式相轉換系統製備成MOF複合膜，濕式相轉換過程中有機連接劑因相轉換驅動於界面相反應形成金屬-有機框架混合物之皮層。
利用MOF前驅物濃度梯度之差異可有效控制金屬-有機框架混合物於分離皮層之厚度與晶體孔隙大小，藉由不同濕式成膜條件之應用，製備出MOF/polysulfone平板膜，可藉由有機連接劑分子種類及濃度加以改變MOF複合膜中之孔隙，MOF內孔因具金屬離子中心而具高親水性，因此具備對水高度之選擇性，另一方面MOF薄膜奈米級微孔隙將可大幅降低水分子穿透薄膜之阻力，使水分子通透過滲透蒸發薄膜通量大幅增加。
所合成之MOF/polysulfone 薄層複合膜將具備對水高度選擇性且具備高通量之分離性能。本論文探討影響MOF 薄層複合膜分離性能因素包含: linker 種類及濃度、相轉換條件及金屬鹽類添加量控制以及金屬鹽類在成膜中是否分散均勻等對複合膜緻密性及分離特性之影響，所得到適當複合膜結構之MOF薄層複合膜將應用於乙醇-水混合液之滲透蒸發分離。

In this research, the blending method was used to prepare a metal-organic framework (MOF)/polysulfone composite membranes. The organic linker and central metal were dissolved in the casting solution and prepared asymmetric membranes by wet phase inversion method. The MOFs can be migrated to the skin layer of asymmetric membrane due to the organic solvent exchanged in phase inversion process.
The concentration and crystal size of MOFs in the separation layer of membrane can be prepared by the gradient concentration of MOF precursor in casting procedure. Different asymmetric composite membranes can be prepared by using the suitable casting conditions in wet phase inversion. The pore size of MOF crystal can be changed by adjusted the concentration of organic linkers. Due to the ionic central in MOF, the high polarity function group contributed the highly hydrophilic property and expected to obtain a high separation performance of dehydration membranes. On the other hand, the pore of MOF crystal in the skin layer will significantly decreased the barrier of permeate and increased the permeation rate of permeates.
The influent factors on the separation performance of composite membrane will be discussed in this investigation, such as type of linker, linker concentration, casting conditions, and dispersion of MOF in the skin layer. The composite membranes will be applied for dehydration of ethanol solution by pervaporation.

目錄
摘要 I
Abstract II
目錄 III
圖目錄 VII
表目錄 XI
第一章、 前言 1
1-1、研究動機 1
1-2、研究目的 3
第二章、 文獻回顧 4
2-1、薄膜定義 4
2-1-1、薄膜特性 4
2-2、薄膜結構 7
2-3、薄膜成型原理 9
2-4、薄膜分離 12
2-5、薄膜製備方法 13
2-6、薄膜過濾方式及運作程序 16
2-6-1、薄膜運作程序 18
2-7、薄膜接觸角原理 20
2-8、滲透蒸發原理 23
2-8-1、滲透蒸發基礎輸送機制 25
2-9、金屬有機框架複合膜(Metal-organic framework MOF)/polysulfone 26
2-9-1、金屬有機框架複合膜(MOF)/ZIF-8、MIL-53 29
2-10、薄膜改質親水化 30
2-10-1、(Metal-organic framework)複合膜，添加改質物：單寧酸 34
第三章、 材料與方法 35
3-1、實驗藥品及氣體 35
3-1-1、高分子鑄膜液材料與實驗藥品 35
3-1-2、薄膜親水化實驗 35
3-1-3、薄膜膨潤化實驗 35
3-1-4、滲透蒸發實驗 35
3-1-5、吸附實驗 36
3-2、實驗儀器及設備 36
3-3、實驗流程 38
3-3-1、鑄膜液配置 40
3-3-2、製備MOFs平板膜(Metal-organic framework) 40
3-3-3、表面接觸角測量儀(Contact Angle) 42
3-3-2、膨潤度測試 43
3-3-3、薄膜吸附測試 44
3-3-4、滲透蒸發測試 45
第四章、 結果與討論 47
4-1、MOF含量對金屬有機框架(MOFs)複合膜表面親疏水性影響 48
4-1-1、ZIF-8複合膜鑄膜液高分子濃度對於接觸角之影響 49
4-1-2、添加不同ZIF-8比例對複合膜接觸角之影響 50
4-1-3、不同類型MOF添加單寧酸對接觸角影響 51
4-2、金屬有機框架(MOFs)複合膜滲透蒸發過程中對膨潤度影響 53
4-2-1、進料液乙醇濃度變化對ZIF-8膨潤度之影響 54
4-2-2、不同乙醇濃度對不同類型MOF膨潤度之影響 55
4-3、金屬有機框架（MOFs）複合膜滲透蒸發之分離探討 59
4-3-1、不同鑄膜液濃度對滲透蒸發之選擇比影響 60
4-3-2、不同比例MOF對ZIF-8複合膜選擇比影響 63
4-3-3、滲透蒸發實驗進料液溫度變化對於ZIF-8複合膜選擇比之影響 64
4-3-4、滲透蒸發實驗進料液溫度變化對於MIL-53複合膜選擇比之影響 78
4-4、進料液濃度及溫度對於MOFs複合膜吸附之影響。 92
第五章、 結論 95
第六章、 參考文獻 96
圖目錄
圖2- 1、（左）對稱型薄膜（右）非對稱型薄 8
圖2- 2、高分子/溶劑/非溶劑三相組成示意圖 11
圖2-3、溶劑/凝聚劑相互擴散示意圖 11
圖2- 4、薄膜過濾示意圖 12
圖2- 5、垂直式過濾與掃流式過濾 17
圖2- 6、掃流式過濾與作用力 17
圖2- 7、薄膜積垢 (a)完全阻塞 (b)標準阻塞 (c)膠羽層/濾餅層阻塞 19
圖2- 8、接觸角原理 20
圖2- 9、Wenzel's Theory 表面圖 22
圖2- 10、Cassie's Theory 表面圖 22
圖2- 11、滲透蒸發-溶液擴散過程 24
圖2- 12、蒸餾分離乙醇/水混合物 24
圖2- 13、MOF種類晶體結構 26
圖2- 14、最佳MOF負載量對複合膜選擇性的影響 27
圖2- 15、通過MMM的非理想滲透物傳輸特性 28
圖2- 16、The channel is constructed of eight homochiral helical chains with18.3Å ×22.4Å of JUC-60 30
圖2- 17、孔洞填充法 31
圖2- 18、界面聚合法 31
圖2- 19、高分子摻合法 32
圖2- 20、化學接枝法 33
圖2- 21、MOF薄膜表面親水化 34
圖3- 1、 MOFs複合膜合成 38
圖3- 2、實驗架構流程圖 39
圖3- 3、製備平板膜 41
圖3- 4、接觸角示意圖 42
圖3- 5、Pervaporation test setup: 46
圖4- 1、ZIF-8複合膜鑄膜液濃度對接觸角影響 49
圖4- 2、添加不同ZIF-8比例對複合膜接觸角之影響 50
圖4- 3、ZIF-8複合膜添加單寧酸對接觸角之影響(鑄膜液濃度26wt%) 52
圖4- 4、MIL-53複合膜添加單寧酸對接觸角之影響(鑄膜液濃度26wt%) 52
圖4- 5、不同含量ZIF-8複合膜在不同乙醇濃度之澎潤度 54
圖4- 6、不同MOF比例ZIF-8型複合膜在不同乙醇濃度下膨潤度之影響 57
圖4- 7、不同MOF比例ZIF-8型複合膜/單寧酸在不同乙醇濃度下膨潤度之影響 57
圖4- 8、不同MOF比例MIL-53型複合膜在不同乙醇濃度膨潤度之影響 58
圖4- 9、不同MOF比例MIL-53型複合膜/單寧酸在不同乙醇濃度膨潤度之影響 58
圖4- 11、未添加ZIF-8應用於滲透蒸發之選擇比(鑄膜液18-21wt%) 62
圖4- 12、添加ZIF-8應用於滲透蒸發之選擇比(鑄膜液18-21wt%) 62
圖4- 13、不同比例MOF對ZIF-8複合膜選擇比影響(鑄膜液濃度21wt%) 63
圖4- 14、溫度15°C ZIF-8複合膜滲透蒸發之選擇比、滲透率 67
圖4- 15、溫度15°C ZIF-8/單寧酸複合膜滲透蒸發之選擇比、滲透率 67
圖4- 16、溫度25°C ZIF-8複合膜滲透蒸發之選擇比、滲透率 71
圖4- 17、溫度25°C ZIF-8/單寧酸複合膜滲透蒸發之選擇比、滲透率 71
圖4- 18、溫度35°C ZIF-8複合膜滲透蒸發之選擇比、滲透率 75
圖4- 19、溫度35°C ZIF-8/單寧酸複合膜滲透蒸發之選擇比、滲透率 75
圖4- 20、不同溫度 ZIF-8複合膜滲透蒸發之選擇比 77
圖4- 21、不同溫度 ZIF-8/單寧酸複合膜滲透蒸發之選擇比 77
圖4- 22、溫度15°C MIL-53複合膜滲透蒸發之選擇比、滲透率 81
圖4- 23、溫度15°C MIL-53/單寧酸複合膜滲透蒸發之選擇比、滲透率 81
圖4- 24、溫度25°C MIL-53複合膜滲透蒸發之選擇比、滲透率 85
圖4- 25、溫度25°C MIL-53/單寧酸複合膜滲透蒸發之選擇比、滲透率 85
圖4- 26、溫度35°C MIL-53複合膜滲透蒸發之選擇比、滲透率 89
圖4- 27、溫度35°C MIL-53/單寧酸複合膜滲透蒸發之選擇比、滲透率 89
圖4- 28、不同溫度MIL-53複合膜滲透蒸發之選擇比 91
圖4- 29、不同溫度MIL-53/單寧酸複合膜滲透蒸發之選擇比 91
圖4- 30、不同進料液濃度對於ZIF-8複合膜吸附之影響 93
圖4- 31、不同進料液濃度對於ZIF-8/單寧酸複合膜吸附之影響 93
圖4- 32、不同進料液濃度對於MIL-53複合膜吸附之影響 94
圖4- 33、不同進料液濃度對於MIL-53/單寧酸複合膜吸附之影響 94

 
表目錄
表2- 1、有機膜和無機膜的比較 6
表4- 1、進料液溫度15°C及ZIF-8，ZIF-8/單寧酸複合膜之差異 66
表4- 2、進料液溫度25°C及ZIF-8，ZIF-8/單寧酸複合膜之差異 70
表4- 3、進料液溫度35°C及ZIF-8，ZIF-8/單寧酸複合膜之差異 74
表4- 4、進料液溫度15°C及MIL-53、MIL-53/單寧酸複合膜之差異 80
表4- 5、進料液溫度25°C及MIL-53，MIL-53/單寧酸複合膜之差異 84
表4- 6、進料液溫度35°C及MIL-53、MIL-53/單寧酸複合膜之差異 88

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