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姓名	方煜馨(Yu-Shin Fang)  查詢紙本館藏	畢業系所	化學學系
論文名稱	電場誘導聚苯醚碸摻雜複合薄膜之研究
相關論文	★ 電場誘導有序排列之高導電度複合固態電解質 ★ 改善鋰離子電池電性之新穎電解液添加劑 ★ 電場誘導高離子導向之混摻高分子固態電解質 ★ 以有機茂金屬觸媒合成sPS/PAMS與sPS/PPMS共聚物及其物性探討 ★ 以有機茂金屬觸媒合成丙烯-原冰烯之COC共聚物及其物性探討 ★ 電致發光電池中電解質的結構與物性探討 ★ 奈米二氧化鈦-固態複合高分子電解質 ★ 交聯型固態高分子電解質 ★ 高分子固態電解質改進高分子發光二極體之光學特性研究 ★ 複合高分子電解質結構與電性之研究 ★ 奈米粒/管二氧化鈦複合高分子電解質之結構探討 ★ 具備電子予體與受體之七環十四烷衍生物的製備及其特性 ★ 超分子發光二極體相容性、分子運動性與光性之研究 ★ 新穎質子交換膜 ★ 原位聚合有機無機複合發光二極體 之分散性及光性研究 ★ 原位聚合固態電解質
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摘要(中)	燃料電池質子交換膜仍有幾個缺點待改善，如(1)高溫失水，使質子導電度因缺乏傳遞介質而損失導電度、(2)燃料竄透，儘管有高的質子導電度也會因嚴重的燃料竄透而無法彰顯其效能、(3)耐久穩定性，薄膜須具有良好的機械與化學穩定性延長使用壽命。同時改進以上缺點是極大的挑戰，但目前仍無完整的方案。 本研究利用具有親水性質之PES添加至sPEEK高分子中，並於外加強電場下鑄造成質子交換膜。研究顯示，經由強電場誘導後sPEEK與PES高分子受到電場極化，薄膜中親水孔道在垂直於薄膜表面的方向形成具有方向性的優先取向結構，而此結構大幅的改善離子導電度。施加電場使更多的磺酸根基團顯露於親水域表面參與質子的運送，也使質子導電度大幅增加。此外，施用電場讓疏水區產生密緻化，降低了薄膜的膨潤率、燃料竄透性及提高其機械強度和化學穩定性。添加有機物PES至sPEEK中所製備的有機複合薄膜，在經電場誘導後，3PES/E之薄膜具有高達7.43×10-2 S/cm的質子導電度，在高溫低濕(80℃、20%RH)環境下仍可保持9.69x10-4 S/cm。製做成MEA之DMFC效能在80℃下可達到170 mW/cm2的輸出功率相較於市售薄膜N117的100 mW/cm2的效果更佳。 本研究指出磺酸化程度為基本條件，但提高質子導電度更有效的方法卻不是提高磺酸化程度，而是在膜材中構建具順向性排列的親水流通管道，更有效的利用磺酸根及便捷的傳輸路徑，如此可以使用較低的含水量以大幅提升質子傳導效率。此一新穎製備薄膜方法優化親水孔道的形貌紋理結構特徵，改善質子交換膜導電度，也同時改進了高溫失水、燃料竄透、耐久穩定性等多項物性，有效解決目前燃料電池膜材開發面臨的兩難窘況，該新穎膜材製備方法也能廣泛應用於各不同再生能源裝置所需膜材之開發。
摘要(英)	There are few drawbacks in fuel cell proton exchange membranes that need implementation. They include: (1) dehydration of water at high-temperature leads to poor conductivity, (2) severe fuel permeability and cross-over suppresses power output; (3) weak membrane strength and insufficient chemical stability for long term operation. Improving upon all these deficiencies is a challenging task in fuel cell membrane development. Proton exchange membrane bears hydrophilic channel saturated with ion conducting medium, water. Ion transport is therefore heavily contingent upon the microstructure of this morphological texture. However, relationships between these structural features with ion conductivity have rarely been discussed. Even fewer are the studies of improvement on ion conductivity by means of tailoring channel morphology. Present research uses external electric field poling to create preferentially ordered channel morphology with high structural integral hydrophobic region in the membrane, has shown to effectively improved all prior-mentioned deficiencies. Validity of this approach is demonstrated in the miscible sPEEK/PES composite processed under electric field. The study has demonstrated that electric poling treatment created membrane bearing preferentially ordered hydrophilic channel morphology and densely packed hydrophobic region. Due to more densely packed amorphous hydrophobic domain, the membrane showed lower degree of swelling in water and methanol, and improved mechanical strength and chemical stability. The composite membrane of 3PES/E shows the proton conductivity up to　7.43x10-2 S/cm. Also at the high temperature and low humidity (80℃, 20%RH) environment can still maintain 9.69x10-4 S/cm. Nearly 60% increase of DMFC power output is observed using this membrane, and the best power density is recorded at 170 mA/cm2 (80℃, 1M Methanol). These results made it clear that although high degree of sulfonation is essential to ion conductivity, it is actually more efficient to elevate ion conductivity through architected hydrophilic channel morphology that makes full utilization of the sulfonate groups and established more direct ion transport path. This approach effectively propelled ion conduction using materials bearing lower degree of sulfonation and resolved the long standing dilemma of fuel cell membrane development. The technique is also beneficial to the development of next generation high performance membrane developments encounter in many renewable energy technologies.
關鍵字(中)	★ 聚二醚酮 ★ 聚苯醚碸 ★ 複合薄膜 ★ 電場誘導	關鍵字(英)
論文目次	中文摘要 i Abstract iii 謝誌 v 目錄 vi 圖目錄 x 表目錄 xiv 重要名詞縮寫對照表 xv 第一章 緒論 1 1-1 前言 1 1-2 燃料電池組成及原理 2 1-3 研究動機 6 第二章 基本原理與文獻回顧 8 2-1 燃料電池質子交換膜介紹 8 2-2 質子交換膜傳遞機制 10 2-3 微結構性質探討 12 2-3-1 Nafion 13 2-3-2 sPEEK 17 2-4 PFSA改良與探討 21 2-4-1 Nafion/小分子化合物複合薄膜 22 2-4-2 Nafion/無機複合薄膜 23 2-5 非PFSA系列 28 2-5-1 碳氫高分子薄膜 28 2-5-2 有機/無機複合高分子薄膜 31 2-5-3 大分子/小分子複合高分子薄膜 31 2-6 電場誘導性質探討 35 2-6-1 裝置設計及原理 35 2-6-2 外加電場於質子交換膜之應用 36 第三章 實驗方法與原理 40 3-1 實驗儀器及技術原理 40 3-1-1 場發射掃描式電子顯微鏡(FE-SEM) 40 3-1-2 示差掃描熱卡計(Differential Scanning Calorimeter, DSC) 41 3-1-3 熱重分析儀(Thermal Gravimetric Analysis, TGA) 41 3-1-4 小角度X光散射(Small angle X-ray scattering, SAXS) 42 3-1-5 薄膜吸水量(Water Uptake)及膨潤率(Swelling) 42 3-1-6 離子交換容量(Ion Exchange Capacity, IEC) 43 3-1-7 複合薄膜機械強度測試 44 3-1-8 化學穩定性測試(Fenton’s test) 45 3-1-9 甲醇竄透率 46 3-1-10 質子導電度測量 47 3-1-11 DMFC單電池效能測試 49 3-2 物質合成及薄膜製備 51 3-2-1 磺酸化聚二醚酮高分子 51 3-2-2 有機複合薄膜之製備 51 3-2-3 外加電場裝置設計 52 3-2-4 市售Nafion117前處理 52 3-3 實驗藥品 53 3-4 樣品命名規則 54 第四章 結果與討論 55 4-1 複合薄膜材料性質與效能分析 56 4-1-1 吸水性、膨潤率與質子導電度之比較 57 4-1-2 熱穩定性分析 59 4-1-3 複合薄膜機械效能測試 61 4-1-4 質子導電度與甲醇竄透比較 62 4-1-5 薄膜選擇性(Selectivity) 63 4-1-6 DMFC單電池測試 64 4-2 外加電場誘導高分子複合薄膜探討及性質分析 66 4-2-1 SEM薄膜微結構影像 66 4-2-2 DSC薄膜保水性質分析 68 4-2-3 SAXS小角度散射微結構 70 4-2-4 IEC離子交換容量 72 4-2-5 吸水性及膨潤率與質子導電度比較 73 4-2-6 複合薄膜機械效能測試 75 4-2-7 化學穩定性測試 76 4-2-8 變溫及變濕質子導電度測試 78 4-2-9 質子導電度與甲醇燃料竄透率比較 81 4-2-10 薄膜選擇性(Selectivity) 82 4-2-11 DMFC單電池效能測試 83 第五章 結論與未來展望 85 5-1 結論 85 5-2 未來展望與研究建議 87 參考文獻 89
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指導教授	諸柏仁(Po-jen Chu)	審核日期	2016-7-25
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