探討酸/鹼高分子質子交換膜在無水狀態之研究

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彭元軍(Yuan-Chun Peng) 查詢紙本館藏

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論文名稱

探討酸/鹼高分子質子交換膜在無水狀態之研究
(Studies of Acid/Base Polymer for Anhydrous Proton Exchange Membrane)

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摘要(中)

直接甲醇燃料電池（Direct Methanol Fuel Cell，DMFC）具備了數個符合未來替代能源需求的優勢，因此被認為是最具開發價值的燃料電池種類之一，其中，質子交換膜為整個燃料電池組中最重要的組件之一，質子交換膜的特性將影響燃料電池未來的應用。具有好的熱穩定性的薄膜可以擴大燃料電池工作的溫度範圍，隨著工作溫度的提高，燃料電池的效能也將大大地改善，但是，在高工作溫度下，無法藉著水分帶動質子導電，因此也需要不同以往的質子傳遞機制。本研究使用不同分子量的酸性高分子PAA（poly(acrylic acid)）和鹼性高分子P4VP（poly(4-vinylpyridine)）經過摻合後，利用酸、鹼官能基之間的作用力—氫鍵和離子鍵作用力，製備成酸/鹼高分子複合物質子交換膜，除了具有良好的熱穩定性外，也建構出新的質子傳遞通道，在新的通道內，酸、鹼官能基因吸引力而相互配對，少數未配對上質子的鹼官能基，可接受周圍傳遞過來的質子，並傳遞至周圍的「proton defect」，這類質子傳遞方式在通道內如同進行「zip-unzip」的行為，利用新的質子傳遞機制且同時具有熱穩性定，即可應用於高溫無水狀態下的燃料電池。

摘要(英)

Direct Methanol Fuel Cells (DMFCs) possessing several advantage that tally with the alternative energy source demand in the future. And it is considered to one kind of the fuel cells which having the most developed values. Among them, the proton exchange membrane is one of the most important component in the whole fuel cell. The characteristics of the proton exchange membrane will influence the applications of the fuel cells in the future. If the membrane with good thermal stability, it can expand the operating temperature of the fuel cell. With the increasing of the operating temperature, the performance of the fuel cells will be improved greatly. However, it is unable to deliver the proton by water molecules under higher operating temperature, so need different proton transition mechanisms.
This research uses the acidic polymer PAA (poly(acrylic acid)) of different molecular weight combined with the basic polymer P4VP (poly(4-vinylpyridine)) and P(4VPcoS). Then the proton exchange membranes were prepared by the hydrogen bonding and ionic bonding interaction between the acidic and basic polymers. Besides having good thermal stability, there is a new proton transition channel in the membranes. Since the interaction between the acid and base, the acidic and basic functional groups matched with each other. Other few basic polymer that not matched with proton could accept the proton transmitted over around, then deliver to proton defect nearby. This kind of proton transition mechanism like proceeding zip-unzip behavior. If the membrane has the new proton conductive mechanism and thermal stability, it could have the opportunity to apply in the fuel cells under high temperature and anhydrous conditions.

關鍵字(中)

★ 直接甲醇燃料電池
★ 酸/鹼高分子複合物
★ 質子交換膜
★ 無水狀態

關鍵字(英)

★ Acid/Base Polymer Complex
★ Proton Exchange Membrane (PEM)
★ anhydrous
★ Direct methanol fuel cell (DMFC)

論文目次

中文摘要 Ⅰ
英文摘要 Ⅱ
目錄 Ⅲ
圖目錄 Ⅷ
表目錄 Ⅸ
第一章緒論 1
1-1前言 1
1-2研究動機 4
第二章文獻回顧 5
2-1引言：為什麼要於高溫下操作？ 6
2-1-1PFSA薄膜與相關技術 6
2-1-2為什麼要高溫的高分子電解質薄膜 12
2-2 PFSA薄膜的修飾 13
2-2-1以不含水的低揮發性溶劑膨潤 14
2-2-2薄型的PFSA強化膜 16
2-2-3和親水氧化物的複合物 17
2-2-4無機固態質子導體複合物薄膜 19
2-3替代的磺酸化高分子薄膜和他們的複合物 21
2-4酸/鹼複合物薄膜 29
第三章實驗技術與儀器原理 33
3-1樣品之製備 33
3-1-1 PAA/P4VP高分子質子交換膜之製備 33
3-1-2實驗藥品 34
3-2傅立葉轉換紅外線光譜儀（FT-IR） 35
3-2-1FT-IR之實驗原理 35
3-2-2FT-IT之操作程序 39
3-3微差掃瞄熱卡計（DSC） 39
3-3-1DSC之實驗原理 39
3-3-2DSC之操作程序 40
3-4熱重量分析儀（TGA） 41
3-4-1TGA之實驗原理 41
3-4-2TGA之操作程序 41
3-5 X-ray繞射儀（X-ray diffraction） 42
3-5-1XRD之實驗原理 42
3-5-2XRD之操作程序 42
3-6高角度環狀暗場掃瞄穿透式電子顯微鏡（HAADF STEM） 43
3-6-1HAADF STEM之實驗原理 43
3-6-2HAADF STEM之操作程序 44
3-7固態核磁共振光譜（Solid State NMR） 44
3-7-1Cross-polarization之簡單介紹 44
3-7-2S.S.NMR之操作程序 46
3-8吸水度（Water Uptale） 46
3-9交流阻抗分析儀（AC Impedance） 46
3-9-1AC Impedance之實驗原理 46
3-9-2AC Impedance之操作程序 57
第四章結果與討論 59
4-1PAA/P4VP 系統 61
4-1-1傅立葉轉換紅外線光譜（FT-IR） 61
4-1-2微差掃瞄熱卡計（DSC） 65
4-1-3 X-ray繞射儀（XRD） 68
4-1-4HAADF STEM 71
4-1-513C 固態核磁共振光譜（13C S.S.NMR） 76
4-1-6吸水度（Water Uptake） 83
4-1-7熱重量分析（TGA） 86
4-1-8交流阻抗儀（AC Impedance） 89
4-2PAA/P4VP-o系統 92
4-3PAA/P(4VPcoS)系統 100
第五章結論與未來展望 106
參考文獻 109

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指導教授

諸柏仁(Peter Po-Jen Chu)

審核日期

2006-7-20

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