熱壓製程參數對膜電極組(MEA)性能之影響

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丁富彬(Fu-Pin Ting) 查詢紙本館藏

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論文名稱

熱壓製程參數對膜電極組(MEA)性能之影響
(The effect of hot press process parameter for MEA performance)

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摘要(中)

本論文採用熱壓製程製備膜電極組(Membrane Electrode Ass-
embly, MEA)，所得MEA先用I-V極化曲線分析該電池之性能。然而，由於MEA之壓降損失不能由極化曲線理解其理由，因此本實驗進一步配合交流頻譜(Electrochemical Impedance Spectroscopy ,EIS) 分析探討電池內部結構各組成單元接觸面之特性。
EIS結果顯示：熱壓製程之溫度、壓力、質子交換膜之厚度與Nafion溶液之負載均影響MEA的性能甚鉅。膜電極組熱壓之最佳溫度為125℃，若溫度＜125℃，則質子交換膜與觸媒顆粒黏合不夠緊密；反之，若溫度＞125℃，則造成觸媒顆粒被質子交換膜過度被覆而失去活性。另一方面，膜電極組熱壓之最佳壓力為50kg/cm2，若壓力＜50kg/cm2，其接觸電阻太高；反之，若壓力＞50kg/cm2，造成質子交換膜與觸媒顆粒間接觸壓合之效果不佳。使用厚度不同之Nafion質子交換膜組成MEA時，以最薄的50.8um(Nafion112)，其阻抗最低；而以最厚的177.8um(Nafion117)，其阻抗值最高，電化學阻抗的高低，主要取決於質子交換傳輸路徑的長短，與催化反應的難易而定。Nafion溶液最佳負載量為1.0mg/cm2，若負載量太少則質子傳導所需網絡不足；若負載過量則觸媒與氣體燃料接觸面積太少，無法進行催化反應。
MEA之最佳操作溫度為60℃；若溫度太低，質傳擴散作用不足，電極反應速率降低；若溫度太高，則造成觸媒迅速老化而降低電極反應速率。
MEA之最佳氣體燃料進給量(陽極/陰極化學計量比為1.5：2.0)，當陰極端計量比減小時，則造成氣體燃料供給不足；而當計量比增大時，則造成氣體燃料與催化劑的接觸時間不足，兩者均不利於MEA的有效操作。

摘要(英)

The paper will use hot press process to produce Membrane Electrode Assembly (MEA), and used I-V polarization curve to analyze the performance of the cell. However, the voltage loss of the MEA can not to explain from polarization curve, therefore the experiment to go a step further used Electrochemical Impedance Spectroscopy (EIS), and analyze the characteristic of contact interface of every component inside cell structure.
Result of EIS to exhibit: the temperature and pressure of hot press process, and the thickness of proton exchange membrane, and the load of Nafion solution that have more effect of MEA performance. The best hot press temperature is 125℃ in MEA, if the temperature<125℃,then proton exchange membrane and catalyst particle can not bonding enough. On the other hand if the temperature>125℃, then catalyst particle will to warp by proton exchange membrane and to lose activity. On the other hand, the best hot press pressure is 50kgf/cm2 in MEA, if the pressure<50kgf/cm2, then the contract resistance is so high. On the other hand if the pressure>50kgf/cm2, then to cause between proton exchange membrane and catalyst particle bonding result not fine. Use proton exchange membrane of different thickness to compose MEA, when 50.8um (Nafion112) that is most thin and impedance is lowest, and 177.8um (Nafion117) that is most thick and impedance is highest. The electrochemical impedance value that major to depend on proton exchange transmission path is long or short, and catalytic reaction is good or bad to decide. The best Nafion solution load quantity is 1.0mg/cm2. If the load quantity is too less, then proton exchange transmission network is not enough. If the load quantity is too much, then the contract area that between catalyst and gas fuel is too less and can not to proceed catalytic reaction.
The best operation temperature is 60℃ in MEA. If the temperature is lowest, then the effect of mass transmission and diffusion is not enough, and electrode reaction rate is to reduce. If the temperature is highest, then to cause catalyst ageing quickly, furthermore reduce electrode reaction rate.
The best gas fuel feed quantity (anode/cathode chemical stoichiometry is 1.5:2.0). When the stoichiometry is reduce in cathode that to cause gas fuel feed is not enough. When the stoichiometry is to increase that to cause the contract time of between gas fuel feed and catalyst are not enough. Both of above condition are not effective operation for MEA.

關鍵字(中)

★ 交流阻抗
★ 熱壓
★ 膜電極組

關鍵字(英)

★ Membrane Electrode Assembly (MEA)
★ hot press
★ Electrochemical Impedance Spectroscopy (EIS)

論文目次

中文摘要 Ⅰ
英文摘要 Ⅲ
誌謝 Ⅴ
目錄 Ⅵ
表目錄 Ⅹ
圖目錄 ⅩⅢ
第一章緒論 1
1.1 研究背景 1
1.2 研究動機與目的 3
第二章質子交換膜燃料電池(PEMFC)之核心膜電極組(MEA) 4
2.1質子交換膜燃料電池(PEMFC)中膜電極組(MEA)之簡介與製作 4
2.1.1 質子交換膜(Proton Exchange Membrane) 4
2.1.2 觸媒層(Catalyst Layer) 6
2.1.3 氣體擴散層(Gas Diffusion Layer, GDL) 8
2.2 膜電極組(MEA)之工作原理與反應機制 9
2.3 膜電極組(MEA)製作 11
2.4 影響膜電極組(MEA)性能之決定性因素 14
第三章質子交換膜燃料電池(PEMFC)中膜電極組(MEA)的研究文獻回顧 16
3.1 電池操作參數相關文獻 16
3.2 膜電極組(MEA)製程相關文獻 18
3.3 交流阻抗分析相關文獻 24
3.4 微觀分析相關文獻 29
第四章燃料電池之分析與理論基礎 31
4.1 直流電極化(I-V)曲線分析 31
4.2 交流電阻抗(EIS)頻譜分析 34
第五章實驗材料設備與檢測 38
5.1 實驗設備與實驗材料 38
5.1.1 實驗設備與分析儀器 38
5.1.2 實驗材料 41
5.2 實驗流程與參數設定 42
5.2.1 適當電池操作條件選定實驗 43
5.2.1.1 電池工作溫度選定實驗 43
5.2.1.2 氣體燃料進給流量選定實驗 43
5.2.2 適當製程參數選定實驗 46
5.2.2.1 熱壓製程參數選定實驗 46
5.2.2.2 質子交換膜厚度選定實驗 47
5.2.2.2 Nafion溶液負載量選定實驗 47
5.3 實驗方法 49
5.3.1 直流電極化(I-V)曲線分析 49
5.3.2 交流電阻抗(EIS)頻譜分析 49
第六章結果 51
6.1 操作參數與膜電極組(MEA)性能之關係 51
6.1.1 電池工作溫度與MEA性能之關係 51
6.1.1.1 直流電極化(I-V)曲線分析 51
6.1.1.2 交流電阻抗(EIS)頻譜分析 52
6.1.2 氣體燃料進給流量與MEA性能之關係 54
6.1.2.1直流電極化(I-V)曲線分析 54
6.1.2.2交流電阻抗(EIS)頻譜分析 55
6.2 製程參數與膜電極組(MEA)性能之關係 56
6.2.1 膜電極組(MEA)之熱壓製程研究 56
6.2.1.1 直流電極化(I-V)曲線分析 56
6.2.1.2 交流電阻抗(EIS)頻譜分析 58
6.2.2 質子交換膜厚度與MEA性能之關係 62
6.2.2.1直流電極化(I-V)曲線分析 62
6.2.2.2交流電阻抗(EIS)頻譜分析 62
6.2.3 Nafion溶液負載量與MEA性能之關係 64
6.2.3.1直流電極化(I-V)曲線分析 64
6.2.3.2交流電阻抗(EIS)頻譜分析 65
6.3 微結構分析之結果 67
第七章討論 70
7.1質子交換膜燃料電池(PEMFC)最佳操作參數之選取 70
7.1.1 電池最佳工作之溫度 70
7.1.2 氣體燃料最佳進給流量 72
7.2 最佳膜電極組(MEA)製程參數之求得 74
7.2.1 最佳膜電極組(MEA)熱壓參數 74
7.2.1.1 熱壓溫度之影響 74
7.2.1.2 熱壓壓力之影響 79
7.2.2 最佳質子交換膜厚度 83
7.2.3 最佳Nafion溶液負載量 86
第八章結論與未來展望 90
8.1 結論 90
8.2 未來展望 91
第九章參考文獻 93

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指導教授

林景崎(Jing-Chie Lin)

審核日期

2006-7-18

推文