臺灣博碩士論文加值系統

質子交換膜燃料電池（PEMFC）的電解質/觸媒/電極三相界面（TPB）特性，是決定電池效能最重要的關鍵。這個三相界面分別在陽極端使氫氣進行氧化反應，讓陰極端的氧氣產生還原反應，並兼具傳輸質子至電解質及傳導電子至電極的功能。所以增加此界面的有效反應面積，或降低電解質/觸媒/電極之間的接觸電阻，對電池效能表現都有正向的幫助。本研究將針對Nafion®117質導膜，利用氧電漿離子轟擊技術來提高表面粗糙度，進而增加三相界面的有效反應面積，並提升觸媒附著性；同時，採用自我呼吸製程來披覆初始觸媒，作為導電層（Conductivity Layer）之用，且讓觸媒能緊密附著在質導膜表面，使三相界面的接觸電阻降低。改質後試片與未經處理的試片比較，經過電漿處理與自我呼吸製程降低燃料電池內阻抗，其原因在於有效降低電荷轉移阻抗。研究中最佳參數為bs-BO2-20 W，有最小的0.45 Ω電荷轉移阻抗、最高的電流密度130 mA/cm2及輸出功率密度41 mW/cm2，相較於bs-N00其電荷轉移阻抗降低0.54 Ω、電流密度增加42 mA/cm2而輸出功率則提升了15 mW/cm2。

The three-phase boundaries（TPB）at the interfaces of electrolyte|catalyst|electrode play an important role in determining the performance of the proton-exchange membrane fuel cells (PEMFC). The electrochemical reactions occurring at the TPB include oxidation in the hydrogen anode site and reduction in the oxygen cathode site. In addition, the transfer of proton to electrolyte and electron to electrode must function well at the interface. Increasing the interface effective area or lowering the charge transfer resistance of the interface have positive effects to the cell performance. In this study, oxygen plasma bombardment was used to increase the surface roughness of Nafion® 117 membrane, and the interface effective area. We also used a self-breathing process to coating the initial Pt/C catalyst layer, which serve as adhesion layer to further reduce the charge transfer resistance of the interface. The results show that the plasma treatments and self-breathing processes were effective in reducing the interface charge transfer resistance, which was 1∼2 order less than the untreated samples. At optimal plasma and self-breathing perimeters, the interface charge transfer resistance as low as 0.54 Ω.

致謝 I
中文摘要 III
Abstract IV
總目錄 V
圖目錄 VIII
表目錄 XII
符號對照表 XIII
第一章 緒論及研究動機 1
1-1 前言 1
1-2 研究動機 4
第二章 理論基礎與文獻回顧 9
2-1 燃料電池簡介 9
2-2 燃料電池的演進發展 9
2-2-1 國內外發展現況 10
2-3 燃料電池之基本原理 12
2-3-1 燃料電池之熱力學探討 14
2-3-2 燃料電池之動力學探討 17
2-3-3 燃料電池之效率探討 27
2-4 交流阻抗分析 29
2-5 文獻回顧 31
第三章 實驗方法與鑑定分析 39
3-1 實驗材料與設備 39
3-1-1 實驗材料 39
3-1-2 實驗設備 39
3-2 實驗方法 40
3-2-1 質導膜前處理 40
3-2-2 以CCP電漿離子轟擊進行質導膜表面改質 40
3-2-3 質導膜之觸媒自我呼吸製程 41
3-2-4 膜電極組件（MEA）之製備 42
3-3 實驗參數代碼 42
3-4 材料鑑定與分析 42
3-4-1 高解析可變真空掃描式電子顯微鏡及能量散佈光譜儀 43
3-4-2 高解析多功能掃描式探針顯微鏡 43
3-4-3 傅立葉轉換紅外線光譜儀 44
3-4-4 化學分析電子能譜儀 44
3-4-5 交流阻抗電化學特性測試 45
3-4-6 燃料電池性能量測 46
第四章 結果與討論 52
4-1 電漿處理質導膜之特性分析 52
4-1-1 表面型態 52
4-1-2 表面官能基 53
4-1-3 表面鍵結型態 54
4-1-4 離子導電度 57
4-2 電漿改質對觸媒披覆之影響 59
4-2-1 表面形貌 59
4-2-2 酸蝕測試 60
4-3 單電池阻抗性質分析 63
4-3-1 電漿處理效應 63
4-3-2 自我呼吸製程效應 65
4-3-2 三相界面性質最佳化 67
4-4 燃料電池性能分析 68
4-4-1 時效測試性質 68
4-4-2 極化曲線效能 69
第五章 結論 113
第六章 未來展望 115
參考文獻 116

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