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研究生:張偉銘
研究生(外文):Wei-Ming Chang
論文名稱:全氟磺酸樹脂質子交換膜電極組觸媒層結構設計及燃料電池性能研究
論文名稱(外文):Perfluorosulfonic acid proton exchange membrane electrode assemblies catalyst layer structure designs and fuel cells performances
指導教授:林秀麗林秀麗引用關係
學位類別:碩士
校院名稱:元智大學
系所名稱:化學工程與材料科學學系
學門:工程學門
學類:綜合工程學類
論文種類:學術論文
論文出版年:2009
畢業學年度:97
語文別:中文
論文頁數:127
中文關鍵詞:全氟磺酸樹脂質子交換膜燃料電池
外文關鍵詞:NafionPerfluorosulfonic acid resinProton exchange membrane fuel cell.
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本研究論文以: methanol/H2O (4/1 g/g) 及ethanol /H2O (4/1 g/g) 混合溶劑分別溶解Nafion,利用注型成膜方法製作Nafion薄膜;及isopropanol/H2O (4/1 g/g) 混合溶劑、N,N’-dimethylacetamide (DMAc) 與N,N’-dimethylformamide (DMF) 溶劑分別混合Nafion、Pt觸媒、及 Pt-C (Pt on carbon powder support) 觸媒製作觸媒溶液。利用上述Nafion 薄膜及觸媒漿料溶液製作膜電組(MEA)。膜電極組結構包括: (a) 傳統 GDL-Pt/C-membrane-Pt/C-GDL 五層結構; (b) GDL-Pt-Pt/C -membrane-Pt/C-Pt-GDL七層結構; (c) GDL-Pt/C-Pt-membrane -Pt-Pt/C-GDL七層結構; (d) GDL-Pt-Pt/C-Pt-membrane-Pt-Pt/C-Pt-GDL九層結構。MEA單電池 i-V 數據及 impedance數據顯示以methanol/H2O及ethanol /H2O 溶液注型成膜的Nafion薄膜質子傳導阻抗低於杜邦公司 Nafion-212 薄膜。而結構 (c) 及結構 (d) 之MEA 較結構 (a) 及結構 (b) 之MEA有較佳的電池性能。
This thesis used methanol/H2O (4/1 g/g) and ethanol/H2O (4/1 g/g) mixed solutions to dissolve Nafion solid respectively. Nafion membranes were prepared by ” solutions casting ”;and isopropanol/H2O (4/1 g/g) mixed solution, N,N’-dimethylacetamide (DMAc) and N,N’-dimethyl -formamide (DMF) solvent were mixed Nafion solid, Pt catalyst and Pt-C (Pt on carbon powder support) to preparing catalyst ink solution. The above-mentioned Nafion membranes and catalyst ink solution were prepared for membrane electrode assemblies (MEA). Membrane electrode assemblies structures included, (a) convention GDL-Pt/C -membrane-Pt/C-GDL five-layers structure, (b) GDL-Pt-Pt/C-membrane -Pt/C-Pt-GDL seven-layers structure, (c) GDL-Pt/C-Pt-membrane-Pt -Pt/C-GDL seven- layers structure, (d) GDL-Pt-Pt/C-Pt-membrane-Pt- Pt/C-Pt-GDL nine- layers structure. The MEA single cell i-V curve data, and impedance data showed that proton conduction of Nafion membrane which were prepared by methanol/H2O and ethanol/H2O solutions casting was lower than Nafion-212 membrane which were prepared by Du Pont Co..The MEA of structures (c) and (d) had much better fuel cells performances than structures (a) and (b).
目錄
摘 要 I
Abstract II
目錄 IV
圖目錄 VII
表目錄 XI
第一章 序論 1
1-1. 前言 1
1-2. 燃料電池簡介 2
1-3. Nafion簡介 4
1-4. Nafion膜之溶解及Nafion /醇水溶液 5
1-5. 膜電極組製作及觸媒層塗佈 9
1-6. 研究目的 12
第二章 實驗方法 15
2-1. 實驗流程 15
2-2. 實驗藥品 16
2-3. 儀器設備 17
2-4. Nafion固體製備 18
2-5. Nafion/MeOH/H2O溶液注型膜材製作 18
2-6. Nafion/EtOH/H2O溶液注型膜材製作 18
2-7. Nafion/MeOH/H2O&Nafion/EtOH/H2O膜材熱處理 19
2-8. 電極製備 19
2-9. 觸媒漿料配製 20
2-10. 觸媒漿料配方 20
2-11. MEA製備 26
2-12. 氮氣吸脫附等溫曲線、表面積 與孔洞特性鑑定 30
2-13. PEMFC單電池性能測試 32
2-14. MEA阻抗(Impedance)測試 34
第三章 結果與討論 35
3-1. 不同觸媒層結構設計對於單電池效能之影響 35
3-1.1 Nafion-125(M)-(a)、(b)、(c)、(d)-DMAc MEA單電池數據 35
3-1.2 Nafion-125(M)-(a)、(b)、(c)、(d)-DMAc MEA Impedance數據 44
3-1.3 Nafion-125(M)-(a)、(b)、(c)、(d)-DMF MEA 單電池數據 53
3-1.4 Nafion-125(M)-(a)、(b)、(c)、(d)-DMF MEA Impedance 數據 61
3-1.5 Nafion-125(E)- (a)、(b)、(c)、(d)-DMAc MEA 單電池數據 68
3-1.6 Nafion-125(E)-(a)、(b)、(c)、(d)-DMAc MEA Impedance 數據 77
3-1.7 Nafion-125(E)-(a)、(b)、(c)、(d)-DMF MEA 單電池數據 86
3-1.8 Nafion-125(E)-(a)、(b)、(c)、(d)-DMF MEA Impedance數據 94
3-2. 三種不同的觸媒漿料溶劑-手工塗佈-對膜電極組單電池性能的影響 102
3-2.1 N212-(a)-三種不同溶劑製備觸媒漿料溶液手工塗佈製作MEA-單電池測試比較 102
3-2.3 三種不同溶劑製備觸媒溶液手工塗佈電極-ASAP分析比較 105
3-2.4 三種不同溶劑製備觸媒溶液手工塗佈電極之表面型態-SEM 106
3-3. 三種不同的觸媒漿料溶劑-超音波塗佈-對膜電極組單電池性能的影響 108
3-3.1 N212-(a)-三種不同溶劑製備觸媒漿料溶液超音波塗佈製作MEA-單電池測試比較 108
3-3.2 N212-(a)-三種不同溶劑製備觸媒漿料溶液超音波塗佈製作MEA- Impedance 數據 109
3-4. 兩種不同觸媒漿料溶劑對膜電極組單電池性能的影響 111
3-4.1 N125(M)-(a)、(b)-兩種不同溶劑製備觸媒漿料溶液手工塗佈製作MEA-單電池測試比較 111
3-4.2 N125(M)-(c)、(d)-兩種不同溶劑製備觸媒漿料溶液手工塗佈製作MEA-單電池測試比較 112
3-4.3 N125(E)-(a)、(b)-兩種不同溶劑製備觸媒漿料溶液手工塗佈製作MEA-單電池測試比較 113
3-4.4 N125(E)-(b)、(c)、(d)-兩種不同溶劑製備觸媒漿料溶液超音波塗佈製作MEA-單電池測試比較 114
第四章 結論 117
第五章 參考文獻 119

圖目錄
圖 1.1 質子交換膜燃料電池構造示意圖 2
圖 1.2 直接甲醇燃料電池構造示意圖 3
圖 1.3 Nafion化學結構式 4
圖 1.4 Nafion醇水溶液中分子聚集示意圖 5
圖 1.5-a Nafion分子在稀釋溶液([Nafion]≦5.0 mg/mL)主鏈的 一次聚集(primary aggregation) 7
圖 1.5-b Nafion分子在較高濃度溶液([Nafion]>5.0 mg/mL)的 一次聚集(primary aggregation) 7
圖 1.5-c 二次離子聚集(secondary ionic aggregation) 8
圖 1.6 觸媒層結構設計 (a)、(b)、(c)、(d)四種。 13
圖 2.1 Nafion/MeOH/H2O溶液注型成膜實驗流程 15
圖 2.2 Nafion/EtOH/H2O溶液注型成膜實驗流程 15
圖 2.3 觸媒層結構設計 (a)、(b)、(c)、(d)四種。 19
圖 2.4 MEA 樣品編號示意 26
圖 2.5 PEMFC電池結構示意圖 32
圖 2.6 三蛇流道 33
圖 2.7 單蛇流道 33
圖 3.1 MEA-N125(M)-(a)-DMAc 單電池測試 36
圖 3.2 MEA-N125(M)-(b)-DMAc 單電池測試 37
圖 3.3 MEA-N125(M)-(c)-DMAc 單電池測試 38
圖 3.4 MEA-N125(M)-(d)-DMAc 單電池測試 39
圖 3.5 MEA-N212-(a)-IPA+H2O 單電池測試 40
圖 3.6 MEA-N212-(a)-DMAc 單電池測試 41
圖 3.7 MEA-N125(M)-(a)、(b)、(c)、(d)-DMAc 單電池數據 42
圖 3.8 MEA-N125(M)-(a)、(b)、(c)、(d)-DMAc 單電池數據 43
圖 3.9 等效模擬電路圖 44
圖 3.10 MEA-N125(M)-(a)-DMAc Impedance 數據 45
圖 3.11 MEA-N125(M)-(b)-DMAc Impedance數據 46
圖 3.12 MEA-N125(M)-(c)-DMAc Impedance數據 47
圖 3.13 MEA-N125(M)-(d)-DMAc Impedance數據 48
圖 3.14 MEA-N212-(a)-IPA+H2O Impedance數據 49
圖 3.15 MEA-N212-(a)-DMAc Impedance 數據 50
圖 3.16 MEA-N125(M)-(a)、(b)、(c)、(d)-DMAc Impedance 數據 51
圖 3.17 MEA-N125(M)-(a)-DMF 單電池測試 54
圖 3.18 MEA-N125(M)-(b)-DMF 單電池測試 55
圖 3.19 MEA-N125(M)-(c)-DMF 單電池測試 56
圖 3.20 MEA-N125(M)-(d)-DMF 單電池測試 57
圖 3.21 MEA-N212-(a)-DMF 單電池測試 58
圖 3.22 MEA-N125(M)- (a)、(b)、(c)、(d)-DMF 單電池數據 59
圖 3.23 MEA-N125(M)- (a)、(b)、(c)、(d)-DMF 單電池數據 60
圖 3.24 MEA-N125(M)-(a)-DMF Impedance 數據 61
圖 3.25 MEA-N125(M)-(b)-DMF Impedance 數據 62
圖 3.26 MEA-N125(M)-(c)-DMF Impedance 數據 63
圖 3.27 MEA-N125(M)-(d)-DMF Impedance 數據 64
圖 3.28 MEA-N212-(a)-DMF Impedance 數據 65
圖 3.29 MEA-N125(M)-(a)、(b)、(c)、(d)-DMF Impedance數據 66
圖 3.30 MEA-N125(E)-(a)-DMAc 單電池測試 68
圖 3.31 MEA-N125(E)-(b)-DMAc 單電池測試 69
圖 3.32 MEA-N125(E)-(c)-DMAc(Ultra) 單電池測試 70
圖 3.33 MEA-N125(E)-(d)-DMAc(Ultra) 單電池測試 71
圖 3.34 MEA-N212-(a)-IPA+H2O(Ultra) 單電池測試 73
圖 3.35 MEA-N212-(a)-DMAc(Ultra) 單電池測試 74
圖 3.36 MEA-N125(E)- (a)、(b)、(c)、(d)-DMAc 單電池數據 75
圖 3.37 MEA-N125(E)- (a)、(b)、(c)、(d)-DMAc 單電池數據 76
圖 3.38 MEA-N125(E)-(a)-DMAc Impedance 數據 77
圖 3.39 MEA-N125(E)-(b)-DMAc Impedance 數據 78
圖 3.40 MEA-N125(E)-(c)-DMAc(Ultra) Impedance 數據 79
圖 3.41 MEA-N125(E)-(d)-DMAc(Ultra) Impedance 數據 80
圖 3.42 MEA-N212-(a)-IPA+H2O(Ultra) Impedance 數據 81
圖 3.43 MEA-N212-(a)-DMAc Impedance(Ultra) 數據 82
圖 3.44 MEA-N125(E)-(a)、(b)、(c)、(d)-DMAc Impedance 數據 84
圖 3.45 MEA-N125(E)-(a)-DMF 單電池測試 86
圖 3.46 MEA-N125(E)-(b)-DMF(Ultra) 單電池測試 87
圖 3.47 MEA-N125(E)-(c)-DMF(Ultra) 單電池測試 88
圖 3.48 MEA-N125(E)-(d)-DMF(Ultra) 單電池測試 89
圖 3.49 MEA-N212-(a)-DMF(Ultra) 單電池測試 91
圖 3.50 MEA-N125(E)- (a)、(b)、(c)、(d)-DMF 單電池數據 92
圖 3.51 MEA-N125(E)- (a)、(b)、(c)、(d)-DMF 單電池數據 93
圖 3.52 MEA-N125(E)-(a)-DMF Impedance數據 94
圖 3.53 MEA-N125(E)-(b)-DMF(Ultra) Impedance 數據 95
圖 3.54 MEA-N125(E)-(c)-DMF(Ultra) Impedance數據 96
圖 3.55 MEA-N125(E)-(d)-DMF(Ultra) Impedance數據 97
圖 3.56 MEA-N212-(a)-DMF(Ultra) Impedance 數據 98
圖 3.57 MEA-N125(E)-(a)、(b)、(c)、(d)-DMF Impedance 數據 100
圖 3.58 N212-(a)-三種不同溶劑手工塗佈製作MEA 單電池數據 102
圖 3.59 N212-(a)-三種不同溶劑手工塗佈製作MEA Impedance 數據 103
圖 3.60 不同溶劑製備觸媒溶液塗佈於碳紙表面 之SEM照片(X1000) 106
圖 3.61 不同溶劑製備觸媒溶液塗佈於碳紙表面 之SEM照片(X10000) 107
圖 3.62 N212-(a)-不同溶劑超音波塗佈製作MEA 單電池數據 108
圖 3.63 N212-(a)-三種不同溶劑超音波塗佈製作MEA Impedance數據 109
圖 3.64 N125(M)-(a)、(b)兩種不同溶劑手工塗佈MEA單電池數據 111
圖 3.65 N125(M)-(c)、(d)兩種不同溶劑手工塗佈MEA單電池數據 112
圖 3.66 N125(E)-(a)、(b)兩種不同溶劑手工塗佈MEA單電池數據 113
圖 3.67 N125(E)-(b)、(c)、(d)兩種不同溶劑超音波塗佈MEA單電池數據 114


表目錄
表 1.1 溶劑及Nafion的溶解參數與介電常數 8
表 2.1 觸媒層各成份含量及相對位置 19
表 3.1 MEA-N125(M)-(a)-DMAc Impedance 數值 45
表 3.2 MEA-N125(M)-(b)-DMAc Impedance 數值 46
表 3.3 MEA-N125(M)-(c)-DMAc Impedance 數值 47
表 3.4 MEA-N125(M)-(d)-DMAc Impedance 數值 48
表 3.5 MEA-N212-(a)-IPA+H2O Impedance 數值 49
表 3.6 MEA-N212-(a)-DMAc Impedance 數值 50
表 3.7 MEA-N125(M)-(a)、(b)、(c)、(d)-DMAc 負載 3 A (i = 120 mA/cm2) Impedance 數值比較 52
表 3.8 MEA-N125(M)-(a)、(b)、(c)、(d)-DMAc 負載 20 A (i = 800 mA/cm2) Impedance 數值比較 52
表 3.9 MEA-N125(M)-(a)-DMF Impedance 數值 62
表 3.10 MEA-N125(M)-(b)-DMAc Impedance 數值 62
表 3.11 MEA-N125(M)-(c)-DMAc Impedance 數值 63
表 3.12 MEA-N125(M)-(d)-DMF Impedance 數值 64
表 3.13 MEA-N212-(a)-DMF Impedance 數值 65
表 3.14 MEA-N125(M)-(a)、(b)、(c)、(d)-DMF 負載 3 A (i = 120 mA/cm2) Impedance 數值比較 67
表 3.15 MEA-N125(M)-(a)、(b)、(c)、(d)-DMF 負載 20 A(i = 800 mA/cm2) Impedance 數值比較 67
表 3.16 MEA-N125(E)-(a)-DMAc Impedance 數值 78
表 3.17 MEA-N125(E)-(b)-DMAc Impedance 數值 78
表 3.18 MEA-N125(E)- (c)-DMAc(Ultra) Impedance 數值 79
表 3.19 MEA-N125(E)-(d)-DMAc(Ultra) Impedance數值 80
表 3.20 MEA-N212-(a)-IPA+H2O(Ultra) Impedance 數值 81
表 3.21 MEA-N212-(a)-DMAc(Ultra) Impedance 數值 82
表 3.22 MEA-N125(E)-(a)、(b)、(c)、(d)-DMAc 負載 2.5 A (i = 100 mA/cm2) Impedance 數值比較 84
表 3.23 MEA-N125(E)-(a)、(b)、(c)、(d)-DMAc 負載 12.5 A (i = 500 mA/cm2) Impedance 數值比較 85
表 3.24 MEA-N125(E)-(a)、(b)、(c)、(d)-DMAc 負載 25 A (i = 1000 mA/cm2) Impedance 數值比較 85
表 3.25 MEA-N125(E)-(a)-DMF Impedance 數值 95
表 3.26 MEA-N125(E)-(b)-DMF(Ultra) Impedance 數值 95
表 3.27 MEA-N125(E)- (c)-DMF(Ultra) Impedance 數值 96
表 3.28 MEA-N125(E)-(d)-DMF(Ultra) Impedance 數值 97
表 3.29 MEA-N212-(a)-DMF(Ultra) Impedance 數值 98
表 3.30 MEA-N125(E)-(a)、(b)、(c)、(d)-DMF 負載2.5 A (i = 100 mA/cm2) Impedance 數值比較 100
表 3.31 MEA-N125(E)-(a)、(b)、(c)、(d)-DMF 負載12.5 A (i = 500 mA/cm2) Impedance 數值比較 101
表 3.32 MEA-N125(E)-(a)、(b)、(c)、(d)-DMF 負載25 A (i = 1000 mA/cm2) Impedance 數值比較 101
表 3.33 N212-(a)-三種不同溶劑手工塗佈製作MEA 負載3 A (i = 120 mA/cm2) Impedance 數值 104
表 3.34 N212-(a)-三種不同溶劑手工塗佈製作MEA 負載20 A (i = 800 mA/cm2) Impedance 數值 104
表3.35三種不同觸媒溶液手工塗佈碳紙表面BET分析數據 (N2吸附量) 105
表3.36三種不同觸媒溶液手工塗佈電極之Pt觸媒重量 及觸媒比表面積 106
表 3.37 N212-(a)-三種不同溶劑超音波塗佈製作MEA 負載2.5 A (i = 100 mA/cm2) Impedance 數值 110
表 3.38 N212-(a)-三種不同溶劑超音波塗佈製作MEA 負載25 A (i = 1000 mA/cm2) Impedance 數值 110
表 3.39 甲醇/水膜材與標準MEA比較 116
表 3.40 乙醇/水膜材與標準MEA比較 116
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