臺灣博碩士論文加值系統

本研究是將PTFE/Nafion複合膜中加入tetraethoxysilane (TEOS)和磷酸鋯Zr(HPO4)2等無機粒子進行改質，以製備PTFE/Nafion-SiO2及PTFE/Nafion-Zr(HPO4)2種複合膜，並進行SEM、EDX、導電度及單電池等性能測試。膜材的導電度與相對濕度及溫度有關， 110~130℃下PTFE/Nafion-Zr(HPO4)2及PTFE/Nafion-Zr(HPO4)2複合膜的導電度介於1.47 ×10-3 ~ 1.75 ×10-3 S/cm，而Nafion212及PTFE/Nafion膜材的導電度介於1.32 ×10-4~ 1.50 ×10-4 S/cm。所製備的複合膜於相對濕度28.8 %~51.7％、溫度110~130℃及氫氣、氧氣皆為300 ml/min條件下進行單電池性能測試，PTFE/Nafion-Zr(HPO4)2複合膜最大功率密度可達600 mA/cm2 ~ 1200 mA/cm2， PTFE/Nafion-SiO2可以達到600 mA/cm2 ~ 800 mA/cm2，而同樣條件下Nafion 212膜材為300 mA/cm2 ~ 600 mA/cm2。由實驗結果顯示PTFE/Nafion複合膜中加入tetraethoxysilane (TEOS)和磷酸鋯Zr(HPO4)2等無機粒子進行改質可提高複合膜單電池操作溫度及性能。
另本研究將1.5 wt%的幾丁聚醣溶液複合上PTFE薄膜，做成PTFE/Chitosan複合膜，並測試複合膜浸泡不同的酸鹼種類製成MEA之燃料電池效能。其中浸漬H2SO4之PTFE/Chitosan複合膜，開路電位可達到0.86V，然而因為膜材本身機械強度及阻抗問題，電流仍無法測出。

PTFE/Nafion-SiO2 and PTFE/Nafion-Zr(HPO4)2 composite membranes were prepared by impregnation of PTFE/Nafion composite membranes into TEOS and Zr(HPO4)2 solutions.
The PTFE/Nafion-SiO2 and PTFE/Nafion-Zr(HPO4)2 composite membranes have higher conductivity than PTFE/Nafion composite membrance of high temperature(above 100℃).
The results showed the performance of H2/O2 PEMFC based on PTFE/Nafion-Zr(HPO4)2 was better than that of H2/O2 PEMFC based on PTFE/Nafion-SiO2. At 110℃~130 ℃and 28.8%~51.7%RH, the current density of PTFE/Nafion-Zr(HPO4)2 composite membranes were 600 mA/cm2~1200 mA/cm2 ; the current density of PTFE/Nafion-SiO2 composite membranes were 600 mA/cm2~800 mA/cm2 . They both higher than the current density of Nafion 212 which was 300 mA/cm2~600 mA/cm2.
PTFE/Chitosan composite membranes were prepared by immersed in 1.5 wt% chitosan solution. Because of the strength and the resistence of the PTFE/Chitosan composite membranes, We can’t analyze the current of the fuel cell.

目 錄
中文摘要 ..................................................................................Ⅰ
英文摘要 ................................................................................ Ⅲ
目錄 ................................................................................ V
圖目錄 .............................................................................. VII
表目錄 ...............................................................................XIII

一、前 言..................................................................................................1
1.1 燃料電池簡介…..…………………….……………………….….…1
1.2 聚四氟乙烯（PTFE）簡介………………………………………….5
1.3 Nafion（全氟磺酸樹酯）簡介………………………………………5
1.4 幾丁聚醣簡介(chitosan)..………………………..…….………….6
1.5 溶膠-凝膠法(sol-gel reaction)…………………....….……….……7
1.6 研究目的.............................................................................................9
1.7 質子交換膜.......................................................................................10


二、實驗方法............................................................................................16
2.1 實驗架構...........................................................................................16
2.2藥品...................................................................................................18
2.3 儀器設備...........................................................................................19
2.4 實驗步驟...........................................................................................20
2.4-1 PTFE/Nafion/TEOS(P/N-Si)複合膜製備.......................................20
2.4-2 PTFE/Nafion-Zr(HPO4)2(P/N-ZP)複合膜製備..............................22
2.4-3 PTFE/Nafion/Chitosan(P/N-C)複合膜製備...................................23
2.4-4不同厚度的PTFE/Nafion-Chitosan (P/N-C)複合膜製備..............24
2.5 膜電極組(MEA)的製作....................................................................26
2.5-1觸媒配方表.....................................................................................26
2.5-2觸媒層漿料製備.............................................................................26
2.5-3 MEA製法.......................................................................................27
2.6 複合膜的性能分析鑑定...................................................................28
2.6-1 SEM觀察PTFE/Nafion、PTFE/Nafion-SiO2複合膜和PTFE/Nafion--Zr(HPO4)2複合膜表面形態.............................................28
2.6-2 PTFE/Nafion、PTFE/Nafion-SiO2複合膜和PTFE/Nafion--Zr(HPO4)2複合膜EDX元素...........................................28
2.6-3導電度的量測.................................................................................28
2.6-4 中高溫PEMFC單電池性能測試..................................................30
2.6-5 中高溫PEMFC單電池性能測試活化步驟..................................31
2.6-6 中高溫高濕度PEMFC單電池性能測試活化步驟......................31

三、實驗結果與討論...............................................................................32
3.1掃瞄式電子顯微鏡(SEM)..................................................................32
3.2能量性X射線顯微(EDX)元素分析.................................................36
3.3 相對濕度之計算...............................................................................45
3.4 Nafion/PTFE/inorganic複合膜中高溫導電度測試之......................47
3.5 中高溫(110℃~130℃)單電池測試之結果......................................48
3.5-1 不同膜材相同測試條件下的單電池性能比較—活化時間2小時..............................................................................................................48
3.5-2不同膜材相同測試條件下的單電池性能比較—活化時間8小時..............................................................................................................53
3.5-3 相同膜材不同濕度條件下的比較結果........................................57
3.6 P/N-C/(PTFE/Nafion-Chitosan)複合膜浸漬5種不同酸鹼溶液之效能測試......................................................................................................62
3.7 掃描式電子顯微鏡(SEM)觀察P/N-C製作MEA結構..................64
3.8 不同厚度P/N-C-S複合膜單電池測試............................................77

四、結 論...............................................................................................77

五、參考文獻...........................................................................................80

六、附錄....................................................................................................90

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