環烯烴聚醚醚酮與聚醚醚酮酮質子傳導膜之開發

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研究生：	許閣倫 Ke-Lun Hsu
論文名稱：	環烯烴聚醚醚酮與聚醚醚酮酮質子傳導膜之開發 Crosslinkable sulfonated poly(ether ketone)s containing norbornene groups as proton exchange membrane
指導教授：	陳銘洲 Ming-chou Chen
口試委員:
學位類別：	碩士 Master
系所名稱：	理學院 - 化學學系 Department of Chemistry
畢業學年度：	96
語文別：	中文
論文頁數：	109
中文關鍵詞：	質子傳導膜、質子導電度、吸水膨潤度、尺寸穩定性、環烯烴、聚醚醚酮、聚醚醚酮酮
外文關鍵詞：	Norbornene, Proton conductivity, Water uptake, SPEEKK, Swelling ratio, SPEEK, Proton exchange membrane
相關次數：	點閱：9 下載：0
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本篇研究重心在於利用有機反應將環烯烴分子導入Sulfonated poly(ether ketone)s主鏈上，合成出一系列帶有環烯烴分子之NB-Ph SPEEK、NB-p-Ph SPEEK與NB-Np SPEEKK，之後再利用環烯烴分子內的雙鍵進行自由基聚合反應來達成交聯之目的，希望藉由這樣的調控能於質子導電度與膜膨潤情形之間取得平衡，得到適合應用於燃料電池之質子交換膜。此系列帶有環烯烴分子之聚合物同時擁有優異的熱穩定性與氧化穩定性，且於80oC 之熱水裡表現出很好的尺寸穩定性，其中NB-Np SPEEKK 於室溫下導電度更高達 7.52 x 10-2 S/cm，統整以上之結果可看出此類帶有環烯烴分子之膜材確實有潛力成為低成本質子交換膜的選擇之一。

A series of crosslinkable sulfonated poly(ether ketone)s containing norbornene groups were synthesized by aromatic nucleophilic substitution reaction . To decrease the swelling of fuel cell membranes , crosslinking of theses polymers by radical polymerization were be tested. These polymers had good thermal and oxidative stability , and good dimensional stability in hot water . The proton conductivity of NB-Np SPEEKK at room temperature is 7.52 x 10-2 S/cm. The results showed these materials containing norbornene groups are possible inexpensive candidate materials for proton exchange membranes in fuel cell applications.

中文摘要................................................Ⅰ
英文摘要................................................Ⅱ
謝誌....................................................Ⅲ
目錄....................................................IV
表目錄................................................VIII
圖目錄..................................................IX
Scheme..................................................XII
Equation...............................................XIII
附錄目錄................................................XIV
第一章 緒論...............................................1
1-1 新時代的替代能源﹕氫能........................ .......2
1-2 燃料電池概述..........................................3
1-3 燃料電池種類..........................................6
第二章 文獻回顧..........................................16
2-1 質子交換膜簡介.......................................17
2-2 質子交換膜種類.......................................20
2-3 研究動機.............................................30
第三章 實驗技術及原理....................................32
3-1 實驗藥品.............................................33
3-1-1 實驗所使用之化學藥品...............................33
3-1-2 實驗所使用之溶劑...................................35
3-1-3 溶劑除水的部分.....................................35
3-2 實驗儀器及技術原理...................................36
3-2-1 核磁共振光譜儀 (Nuclear Magnetic Resonance)........36
3-2-2 熱重量分析儀 (Thermal Gravimetric Analyzer)........37
3-2-3 微差熱掃描卡計 (Differential Scanning Calorimeter).37
3-2-4 交流阻抗儀 (Alternating Current Impedance).........38
3-2-5 吸水膨潤比 (Water Uptake) 與尺寸變化率 (Swelling Ratio)...................................................40
3-2-6 離子交換容量 (Ion Exchange Capacity；IEC)..........41
3-2-7 薄膜氧化穩定性測試 (Fenton’s Test)................42
3-3 薄膜的製備...........................................42
3-4 薄膜的酸化................................... .......43
3-5 合成步驟....................................... .....44
3-5-1 NB-quinone (1) 的合成......................... ....44
3-5-2 NB-ph-diOAc (2) 的合成.............................45
3-5-3 NB-ph-diOH (3) 的合成..............................46
3-5-4 CH3-ph-quinone (4) 的合成..........................47
3-5-5 CH3-ph-diOH (5) 的合成.............................48
3-5-6 Sodium 5,5’-carbonylbis(2-fluorobenzenesulfonate) (6)的合成................................................49
3-5-7 2-Phenylhydroquinone-5-sulfonic acid monosodium salt (7)的合成................................................50
3-5-8 NB-Ph SPEEK (8) 的合成.............................51
3-5-9 NB-p-Ph SPEEK (9) 的合成.................... ......52
3-5-10 NB-Np SPEEKK (10) 的合成..........................53
第四章 結果與討論........................................54
4-1 1H 核磁共振光譜儀 (1H NMR) ..........................55
4-2 熱重量分析儀 (TGA....................................61
4-3 吸水膨潤比 (WU) 與尺寸變化率 (SW)....................67
4-4 微差掃瞄熱卡計 (DSC) 分析............................72
4-5 氧化穩定性分析 (Fenton’s Test.......................75
4-6 交流阻抗儀 (AC Impedance) 分析.......................77
第五章 結論..............................................80
參考文獻.................................................83
附錄.....................................................88

                                

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