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研究生： 郭易宣
Guo, Yi-Hsuan
論文名稱： 一百瓦磷酸燃料電池系統及膜電極組優化
Establishing a 100W phosphoric acid fuel cell system and ameliorating its membrane electrode assembly
指導教授： 曾繁根
Tseng, Fan-Gang
口試委員: 王本誠
Wang, Pen-Cheng
薛康琳
Hsueh, Kan-Lin
學位類別： 碩士
Master
系所名稱： 原子科學院 - 工程與系統科學系
Department of Engineering and System Science
論文出版年： 2019
畢業學年度： 107
語文別： 中文
論文頁數： 81
中文關鍵詞： 燃料電池 、氫能 、磷酸燃料電池 、質子交換膜
外文關鍵詞： fuel cell, hydrogen energy, phosphoric acid fuel cell, proton exchange membrane
相關次數： 點閱：2  下載：0 
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    • 為了將實驗成果商業化，本研究方向為將本研究室現有的單電池系統改進並規模化，配合本研究室前端甲醇重組器，結合具有較佳抗一氧化碳能力且操作溫度接近重組器的磷酸燃料電池作為發電系統。本研究所使用的磷酸燃料電池質子交換膜為聚苯並咪唑(PBI)，PBI有需多特性，包括熱穩定性，化學穩定性，最特別的是幾乎無電滲拉力，亦即質子在膜內傳遞時，不會將水分子由陽極拖至陰極，此使得在高溫操作下即使無加濕系統，電池系統也不會脫水。
    　　為了大幅縮減製程的時間，電極製作將由原本的噴塗製程改成線棒塗布，本研究中線棒塗佈使用之觸媒漿料，以丁醇作為溶劑配置，並利用特定濕膜厚度之線棒進行塗佈，熱處理後可得微孔層碳黑乘載量2 mg/cm2，觸媒層鉑承載量0.25 mg/cm2，並於170 ℃通以氫氣及氧氣，進行反應面積1 cm2之單電池測試，在電流密度2.798 A/cm2下，可得最高功率密度830 mW/cm2，單位鉑產能更高達3320 mW/mg，觸媒使用率增為原噴塗製程的3倍左右。
    在長效方面，皆操作於定電流密度0.2 A/cm2，170 ℃，除了含微孔層的單層線棒塗佈電極，線棒塗佈所得電極皆比噴塗更為出色穩定。線棒塗佈之雙層觸媒層電極(鉑承載量0.8 mg/cm2)，雖然效能並無顯著提升，然而最高功率劣化速率(每小時0.264 %)卻有約兩倍多的改善。
    　　利用線棒塗佈所得之電極，對反應面積放大作單電池測試之分析。陰陽極分別為空氣及氫氣，於170 ℃操作下，反應面積25 cm2電極所得最高功率密度僅有1 cm2電極之56 %。由極化曲線可知，效能差異主要來自歐姆阻抗，推測施加熱壓壓力太小，以致膜電極組無法緊密貼合。

    For the purpose of commercializing our research, this study is aiming for improving our single cell performance and scale it up. To meet the demands of good carbon monoxide tolerance and high operation temperature for our front-end methanol reforming system, phosphoric acid fuel cell (PAFC) is chosen as our power source.
    In the study, polybenzimidazole (PBI) is introduced to our PAFC as the electrolyte membrane. PBI features good thermal and good chemical stability, and especially no electroosmotic force, which means H2O molecules won’t be dragged from anode to cathode as fuel cell operating. In this case, even without humidification system, cell system won’t dehydrate at high operation temperature (120 ~ 170 ℃).
    To accelerate our electrode manufacturing process, bar coating process is adopted to replace our old spray coating process. In the new process, I take 1-butanol as the solvent of catalyst ink, and use bars with specific wet-film thickness to coat microporous layer (MPL) and catalyst layer (CL) onto carbon clothes. After heat treatment, we can get carbon black loading of 2 mg/cm2 on MPL and Pt loading of 0.25 mg/cm2 on CL. With sufficient hydrogen and oxygen supplied, the peak power density of the electrode is 830 mW/cm2 at 170 ℃, and power per unit Pt is extremely high as 3320 mW/mg which is two times more than that of spray-coating electrode.
    For long-term tests, every cell is operated under constant current density of 0.2 A/cm2 at 170 ℃. Electrodes made by bar coating outperform those made by spray coating. Although Electrodes made by bar coating with 2-catalyst layers (Pt loading 0.8 mg/cm2) show almost no improvement on performance, peak power degradation rate (0.264 % per hour) reduces by more than two times.
    Bar coating technique is applied to analyze the scaling-up of electrode active area. Air and hydrogen are sent to the cathode and the anode respectively in the experiment. At 170 ℃, 25 cm2 electrodes’ peak power density is only 56 % as high as 1 cm2 electrodes’. The difference is mainly from Ohmic resistance, because too small hot press pressure cannot make membrane electrode assembly (MEA) combined tightly.

    總目錄 摘要...............i Abstract...............ii 圖目錄...............vii 表目錄...............xi 第一章 緒論...............1 1-1 前言...............1 1-2 燃料電池簡介...............1 1-3 燃料電池種類與原理...............3 1-3-1 磷酸燃料電池(Phosphoric Acid Fuel Cell, PAFC)...............4 1-3-2 質子交換膜燃料電池(Proton Exchange Membrane Fuel Cell, PEMFC)...............5 1-3-3 鹼性燃料電池(Alkaline Fuel Cell, AFC)...............6 1-3-4 熔融碳酸鹽燃料電池(Molten Carbonate Fuel Cell, MCFC)...............7 1-3-5 固體氧化物燃料電池(Solid Oxide Fuel Cell, SOFC)...............8 1-3-6 直接甲醇燃料電池(Direct Methanol Fuel Cell, DMFC)...............9 1-3-7 甲醇重組式燃料電池(Reformed Methanol Fuel Cell, RMFC)...............9 1-4 研究動機...............12 第二章 基本原理與文獻回顧...............13 2-1 磷酸燃料電池構造...............13 2-1-1 電流收集層與流道...............13 2-1-2 氣體擴散層...............15 2-1-3 觸媒層...............16 2-1-4 質子交換膜...............17 2-1-5 氣密用墊片...............18 2-2 燃料電池理論...............18 2-2-1 電化學熱力學...............18 2-2-2 電化學動力學...............20 2-3 磷酸燃料電池中質子交換膜研究...............22 2-3-1 玻璃纖維與聚四氟乙烯複合膜...............30 2-3-2 玻璃纖維與氧化石墨烯複合膜...............33 2-3-3 鹼性二氧化鈦/PBI複合膜...............35 2-4 氣體擴散層與觸媒層的研究...............38 2-4-1 觸媒劣化...............42 2-5 磷酸燃料電池堆可靠性及耐久性...............44 第三章 實驗方法...............48 3-1 實驗流程...............48 3-2 實驗藥品與設備...............48 3-2-1 實驗藥品、耗材...............48 3-2-2 實驗用氣體...............49 3-2-3 實驗設備...............49 3-2-4 分析儀器...............50 3-3 磷酸燃料電池性能測試...............50 3-3-1 氣體擴散層、觸媒層及電解質膜的製備...............50 3-3-2 膜電極組製備...............52 3-3-3 燃料電池測試...............52 3-4 循環伏安法...............54 第四章 結果與討論...............56 4-1 線棒塗佈分析...............56 4-1-1 線棒塗佈之溶劑選擇...............56 4-1-2 丁醇為溶劑之不同配比測試結果...............59 4-1-3 噴塗與線棒塗佈所得電極之比較...............61 4-1-4 微孔層引入電極中...............64 4-1-5 提升白金程載量...............69 4-2 電極反應面積放大...............71 第五章 結論...............73 第六章 未來展望...............74 參考文獻...............75

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