臺灣博碩士論文加值系統

本論文合成Polybenzimidazole (PBI)及PBI衍生物Butyl sulfonated Polybutylimidazole (PBI-BS)。利用具有微孔洞的Poly tetra fluoro ethylene (PTFE)膜為支撐物，補強PBI及PBI/PBI-BS (8/2 g/g)摻合物，製備PBI/PTFE複合膜及PBI/PBI-BS/PTFE複合膜。我們利用SEM (Scanning Electron Microscope)觀察膜材表面以及截面的結構、TGA (Thermogravimetric analysis)分析膜材熱穩定性。並將PBI/PTFE及PBI/PBI-BS/PTFE此兩種複合膜材製作成膜電極組 (MEA)，分別在160 ℃及定電流i = 200 mA/cm2進行H2/O2單電池的400小時及100小時的長時間測試。在長時間的操作過程中，每12小時分別測定單電池的i-V曲線及以AC-impedance來測試膜材和觸媒的阻抗值。最後以FE-SEM觀察長時間操作實驗前及實驗後MEA之形態差異。

In this study, we synthesized polybenzimidazole (PBI) and its derivative butyl sulfonated polybenzimidazle (PBI-BS).The porous poly tetra fluoro ethylene (PTFE) was used as supporting membranes to reinforce PBI and PBI/PBI-BS (8/2 g/g) blend to prepare PBI/PTFE and PBI/PBI-BS/PTFE composite membranes. These two composite membranes were used to prepare membrane electrode assemblies (MEA). We performed 400 hr H2/O2 life test on PBI/PTFE MEA and 100 hr test on PBI/PBI-BS/PTFE MEA at 160 ℃ with a current density
i = 200 mA/cm2. During long time life test, the i-V curve and AC-impedance measurements of MEAs were performed every 12 hr.

摘要 I
目錄 III
圖目錄 V
表目錄 VII
第一章 序論 1
1.1 前言 1
1.2 燃料電池簡介 3
1.3 質子交換膜簡介 4
1.4 聚苯咪唑 (Polybenzimidazole，PBI)的合成及其在燃料電池之應用 7
1.4.1 PBI的合成 7
1.4.2 PBI在燃料電池上的應用 8
1.4.3 PBI改質薄膜 9
1.4.4 PBI與磺酸化高分子摻合膜 10
1.5 PTFE為基材之複合膜於燃料電池上的應用 11
1.5.1 聚四氟乙烯(PTFE)簡介 11
1.5.2 PBI/PTFE複合膜 12
1.6 研究目的 14
第二章 實驗 15
2.1 實驗架構 15
2.2 實驗藥品 15
2.2 實驗藥品 16
2.3 儀器設備 17
2.4 PBI及PBI-BS的合成及基本鑑定 18
2.4.1 PBI合成 18
2.4.2 PBI-BS合成 19
2.4.3 霍式紅外光譜儀(FTIR)結構鑑定 20
2.4.4 PBI固有黏度測定 20
2.4.5 PBI-BS元素分析儀(EA)性質分析 20
2.5 PBI/PTFE及PBI/PBI-BS/PTFE複合薄膜製備 21
2.5.1 PBI/PTFE複合薄膜製備：注膜法 21
2.5.2 PBI/PTFE薄膜製備：塗佈法 22
2.5.3 PBI/PBI-BS/PTFE薄膜製備：塗佈法 23
2.6 質子交換膜分析鑑定 25
2.6.1 SEM觀察薄膜表面形態 25
2.6.2 TGA熱穩定性分析 25
2.6.3 複合膜組成成份測量 25
2.6.4 含酸率測量 25
2.7 MEA製備 26
2.7.1 電極製備 26
2.7.2 MEA塗佈壓合 26
2.8 質子交換膜燃料電池(PEMFC)高溫長時間測試 27
2.8.1 單電池組裝 29
2.8.2 Impedance量測 (Chino) 29
2.8.3 陰極排水之pH量測 30
2.8.4 實驗前後膜電極組(MEA)SEM、EDX截面分析 30
第三章 結果與討論 31
3.1 PBI合成時間、溫度記錄 31
3.2 PBI及PBI-BS結構鑑定 33
3.2.1 PBI霍式紅外光譜儀(FTIR)分析 33
3.2.2 PBI固有黏度(inherent viscosity)測定 34
3.2.3 PBI-BS霍式紅外光譜儀(FTIR)分析 35
3.2.4 PBI-BS元素分析（EA）鑑定 36
3.3 複合膜之SEM分析鑑定 37
3.3.1 PBI/PTFE 複合膜SEM分析鑑定 37
3.3.2 PBI/PBI-BS/PTFE 複合膜SEM分析鑑定 37
3.4 複合膜組成成份 44
3.5 複合膜熱重分析儀(TGA)測試 45
3.6 PBI/PTFE複合膜(PEMFC)高溫長時間操作測試 47
3.6.1 PBI/PTFE複合膜400小時長時間操作測試 47
3.6.2 PBI/PTFE複合膜400小時長時間測試實驗前及實驗後膜電極組 (MEA)SEM、EDX截面分析 54
3.6.3 PBI/PTFE複合膜100小時加速老化-start/stop循環測試 56
3.7 PBI/PBI-BS/PTFE複合膜(PEMFC)高溫長時間操作測試 61
3.7.1 PBI/PBI-BS/PTFE複合膜100小時長時間操作測試 61
3.7.2 PBI/PBI-BS/PTFE複合膜100小時長時間測試實驗前及實驗後膜電極(MEA)SEM、EDX截面分析 67
第四章 結論 69
第五章 未來工作及建議 70
第六章 參考文獻 71
附錄 78

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