新型四胺單體與聚苯并咪唑之合成及在高溫型質子交換膜燃料電池之應用

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研究生：	林凡傑 FAN-JIE - LIN
論文名稱：	新型四胺單體與聚苯并咪唑之合成及在高溫型質子交換膜燃料電池之應用 Synthesis and Characterization of Novel Tetraamine Monomers and Polybenzimidazoles for High Temperature Proton Exchange Membrane Fuel Cell Applications
指導教授：	陳志堅 Jyh-Chien Chen
口試委員:	劉貴生 Guey-Sheng Liou 蕭勝輝 Sheng-Huei Hsiao 游進陽 Chin-Yang Yu
學位類別：	碩士 Master
系所名稱：	工程學院 - 材料科學與工程系 Department of Materials Science and Engineering
論文出版年：	2017
畢業學年度：	105
語文別：	中文
論文頁數：	94
中文關鍵詞：	四胺、聚苯并咪唑、質子交換膜燃料電池、質子傳導率
外文關鍵詞：	tetraamine, polybenzimidazole, proton exchange membrane fuel cell, proton conductivity
相關次數：	點閱：395 下載：1
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上一筆

本研究利用三種不同的單體反應得到三種不同官能基之四胺單體以此三種四胺單體分別與二酸聚合出聚苯并咪唑P1~P3。但P3由於關環不完全，無法進行後續比較。P1及P2之固有黏度(inherent viscosity)分別為3.2及2.9 dL/g，且皆成功以溶液澆鑄法塗佈成可饒式的薄膜。P1及P2展現出良好的熱化學穩定性。P1 及 P2 薄膜在室溫下浸泡於不同濃度的磷酸(85、 80、 75 %)後展現出良好的PU。P1與P2在摻雜量最大下，拉伸強度分別為 24.4 和 17.0 MPa。P1及P2薄膜在160 ℃下進行全電池測試，比m-PBI 的 573 mW/cm2還高，證實聚苯并咪唑 P1 及 P2 薄膜可應用於質子交換膜燃料電池。

Three novel tetraamines were synthesized via several steps three different compound. Novel polybenzimidazoles P1~P3 were prepared
from OBA and monomer (5), (10) and (14), respectively. P3 could not be characterized because ofincompleted cyclization. The structures of P1 and P2 were characterized by 1H-NMRand FTIR. The inherent viscosity of P1 and P2, measured in methanesulfonic acid at35 ℃ and 0.2 g/dL, were 3.2 and 2.9 dL/g, respectively. P1 and P2 could be prepared as transparent, flexible, and tough membranes by solution casting. P1 and P2 show
outstanding thermal and oxidative stability. When P1 and P2 membranes were immersed in differentconcentrations of phosphoric acid (85, 80 and 75 %) at room temperature, P1 and P2 show good phosphoric acid uptake (PU, %), respectively. The tensile strength of P1 and P2 membranes
was 24.4 and 17.0 MPa when PU were achieve maxium, respectively. For single fuel cell test at 160 ℃, the peak power density of P1 and P2 are higher than thatof m-PBI at 291% PU (573 mW/cm2). It shows that P1 and P2 are promising proton exchange membranes for HT-PEMFC applications.

目錄
中文摘要 ......................................................................................................................................................... I
ABSTRACT ..................................................................................................................................................II
致謝................................................................................................................................................................IV
目錄................................................................................................................................................................. V
FIGURE 索引 ............................................................................................................................................ VII
SCHEME 索引 .............................................................................................................................................X
TABLE 索引 ............................................................................................................................................... XI
第一章 緒論..............................................................................................................................................1
1.1 前言..............................................................................................................................................1
1.2 氫能..............................................................................................................................................2
1.3 燃料電池分類 .............................................................................................................................3
1.4 PEMFC 簡介 ...............................................................................................................................6
1.4.1 PEMFC 之發電原理...................................................................................................................6
1.4.2 PEMFC 之結構...........................................................................................................................7
1.4.3 PEMFC 介紹 ............................................................................................................................ 10
1.4.4 HT-PEMFC 介紹...................................................................................................................... 12
第二章 PBI文獻回顧 .......................................................................................................................... 14
2.1 PBI 的簡介............................................................................................................................... 14
2.2 PBI 之聚合方法....................................................................................................................... 19
2.3 聚苯并咪唑薄膜之製備 ......................................................................................................... 21
2.4 磷酸摻雜 PBI........................................................................................................................... 22
2.5 氧化安定性 .............................................................................................................................. 27
2.6 含氟 PBI................................................................................................................................... 29
2.7 研究動機與目的...................................................................................................................... 32
第三章 實驗........................................................................................................................................... 34
3.1 實驗儀器 .................................................................................................................................. 34
3.2 實驗藥品 .................................................................................................................................. 35
3.3 單體合成 .................................................................................................................................. 37
3.4 新型聚苯并咪唑之聚合 ......................................................................................................... 45
3.5 聚苯并咪唑薄膜之製備方法................................................................................................. 47
3.6 膜電極組(MEMBRANE ELECTRODE ASSEMBLY, MEA)之製備 .............................................. 48
第四章 結果與討論 .............................................................................................................................. 49
4.1 單體合成與表徵...................................................................................................................... 49
4.2 聚苯并咪唑之合成.................................................................................................................. 65
4.3 聚苯并咪唑之氫核磁共振圖譜及紅外線光譜.................................................................... 68
4.4 聚苯并咪唑之分子量與溶解度............................................................................................. 70
4.5 聚苯并咪唑之熱學性質 ......................................................................................................... 72
4.6 聚苯并咪唑之氧化安定性與吸水率..................................................................................... 74
4.7 聚苯并咪唑之磷酸摻雜能力 ................................................................................................. 78
4.8 聚苯并咪唑之機械強度及尺寸安定性 ................................................................................ 81
4.9 質子傳導率測試...................................................................................................................... 83
4.10 質子交換膜燃料電池測試 ..................................................................................................... 86
第五章 結論........................................................................................................................................... 91
參考文獻 ...................................................................................................................................................... 92
                                

1. 李代廣 , 氫能與氫能汽車. 化學工業出版社: 2009.
2. Schools, A. https://schools.aglasem.com/5638 (accessed Dec 28).
3. 名洋科技 http://www.cvtweb.com.tw/newsshow.aspx?myid=52&typee=2
(accessed Dec 28).
4. Dupuis, A.-C., Prog. Mater Sci. 2011, 56, 289.
5. Kraytsberg, A.; Ein-Eli, Y., Energy Fuels 2014, 28, 7303.
6. Zhang, H.; Shen, P. K., Chem. Rev. 2012, 112, 2780.
7. Guo, Q.; N. Pintauro, P.; Tang, H.; O'Connor, S., J. Membr. Sci. 1999, 154, 175.
8. Asensio, J. A.; Sánchez, E. M.; Gómez-Romero, P., Chem. Soc. Rev. 2010, 39,
3210.
9. Appleby, A. J.; Foulkes, F. R., Fuel Cell Handbook. Van Nostrand Reinhold:
1989.
10. Larminie, J.; Dicks, A., Fuel Cell Systams Explained. John Wiley & Son Ltd:
2003.
11. Li, Q.; He, R.; Jensen, J. O.; Bjerrum, N. J., Chem. Mater. 2003, 15, 4896.
12. Zhang, Y.; Litt, M.; Savinell, R. F.; Wainright, J. S., Polym. Prepr. 1999, 40, 480.
13. Kim, S.-K.; Kim, T.-H.; Jung, J.-W.; Lee, J.-C., Polymer 2009, 50, 3495.
14. Kumbharkar, S. C.; Islam, M. N.; Potrekar, R. A.; Kharul, U. K., Polymer 2009,
50, 1403.
15. Li, Q.; Jensen, J. O.; Savinell, R. F.; Bjerrum, N. J., Prog. Polym. Sci. 2009, 34,
449.
16. Potrekar, R. A.; Kulkarni, M. P.; Kulkarni, R. A.; Vernekar, S. P., J. Polym. Sci.,
Part A: Polym. Chem. 2009, 47, 2289.
17. Chen, J.-C.; Chen, P.-Y.; Liu, Y.-C.; Chen, K.-H., J. Membr. Sci. 2016, 513, 270.
18. 黃靖穎; 劉政宏; 王文琳, Journal of Taiwan Energy 2015, 2, 39.
19. Bouchet, R.; Siebert, E., Solid State Ionics 1999, 118, 287.
20. Yang, J.; Li, Q.; Cleemann, L. N.; Xu, C.; Jensen, J. O.; Pan, C.; Bjerrum, N. J.;
He, R., J. Mater. Chem. 2012, 22, 11185.
21. Wainright, J. S.; Wang, J. T.; Weng, D.; Savinell, R. F.; Litt, M., J. Electrochem.
Soc. 1995, 142, L121.
22. Asensio, J. A.; Borrós, S.; Gómez-Romero, P., J. Electrochem. Soc. 2004, 151,
A304.
23. He, R.; Li, Q.; Bach, A.; Jensen, J. O.; Bjerrum, N. J., J. Membr. Sci. 2006, 277,
38.
24. Li, Q.; Hjuler, H. A.; Bjerrum, N. J., J. Appl. Electrochem. 2001, 32, 773.
25. Xiao, L.; Zhang, H.; Scanlon, E.; Ramanathan, L. S.; Choe, E. -W.; Rogers, D.;
93
Apple, T.; Benicewicz, B. C., Chem. Mater. 2005, 17, 5328.
26. Ma, Y.-L.; Wainright, J. S.; Litt, M. H.; Savinell, R. F., J. Electrochem. Soc. 2004,
151, A8.
27. Pu, H.; Liu, G., Polym. Int. 2005, 54, 175.
28. Kumbharkar, S. C.; Karadkar, P. B.; Kharul, U. K., J. Membr. Sci. 2006, 286, 161.
29. Sannigrahi, A.; Arunbabu, D.; Sankar, R. M.; Jana, T., J. Phys. Chem. B 2007, 111,
12124.
30. Földes, E.; Fekete, E.; Karasz, F. E.; Pukánszky, B., Polymer 2000, 41, 975.
31. Liang, K.; Bánhegyi, G.; Karasz, F. E.; MacKnight, W. J., J. Polym. Sci., Part B:
Polym. Phys. 1991, 29, 649.
32. Qing, S.; Huang, W.; Yan, D., Eur. Polym. J. 2005, 41, 1589.
33. Saegusa, Y.; Horikiri, M.; Nakamura, S., Macromol. Chem. Phys. 1997, 198, 619.
34. Li, X.; Qian, G.; Chen, X.; Benicewicz, B. C., Fuel Cells 2013, 13, 832.
35. Li, X.; Chen, X.; Benicewicz, B. C., J. Power Sources 2013, 243, 796.
36. Vogel, H.; Marvel, C. S., J. Polym. Sci. 1961, 50, 511.
37. Iwakura, Y.; Uno, K.; Imai, Y., J. Polym. Sci., Part A: Gen. Pap. 1964, 2, 2605.
38. Eaton, P. E.; Carlson, G. R.; Lee, J. T., J. Org. Chem. 1973, 38, 4071.
39. Schechter, A.; Savinell, R. F., Solid State Ionics 2002, 147, 181.
40. Hughes, C. E.; Haufe, S.; Angerstein, B.; Kalim, R.; Mähr, U.; Reiche, A.; Baldus,
M., J. Phys. Chem. B 2004, 108, 13626.
41. Li, Q.; He, R.; Jensen, J. O.; Bjerrum, N. J., Fuel Cells 2004, 4, 147.
42. Carollo, A.; Quartarone, E.; Tomasi, C.; Mustarelli, P.; Belotti, F.; Magistris, A.;
Maestroni, F.; Parachini, M.; Garlaschelli, L.; Righetti, P. P., J. Power Sources
2006, 160, 175.
43. Leykin, A. Y.; Askadskii, A. A.; Vasilev, V. G.; Rusanov, A. L., J. Membr. Sci.
2010, 347, 69.
44. A. Perry, K.; L. More, K.; Andrew Payzant, E.; Meisner, R. A.; Sumpter, B. G.;
Benicewicz, B. C., J. Polym. Sci., Part B: Polym. Phys. 2014, 52, 26.
45. Teranishi, K.; Kawata, K.; Tsushima, S.; Hirai, S., Electrochem. Solid-State Lett.
2006, 9, A475.
46. Panchenko, A.; Dilger, H.; Möller, E.; Sixt, T.; Roduner, E., J. Power Sources
2004, 127, 325.
47. Chang, Z.; Pu, H.; Wan, D.; Liu, L.; Yuan, J.; Yang, Z., Polym. Degrad. Stab.
2009, 94, 1206.
48. Wang, S.; Zhang, G.; Han, M.; Li, H.; Zhang, Y.; Ni, J.; Ma, W.; Li, M.; Wang, J.;
Liu, Z.; Zhang, L.; Na, H., Int. J. Hydrogen Energy 2011, 36, 8412.
49. O'Hagan, D., Chem. Soc. Rev. 2008, 37, 308.
50. Qian, G.; Benicewicz, B. C., J. Polym. Sci., Part A: Polym. Chem. 2009, 47,
94
4064.
51. Chen, J.-C.; Chen, P.-Y.; Lee, S.-W.; Liou, G.-L.; Chen, C.-J.; Lan, Y.-H.; Chen,
K.-H., React. Funct. Polym. 2016, 108, 122.
52. Qian, G.; Smith Jr, D. W.; Benicewicz, B. C., Polymer 2009, 50, 3911.
53. Guan, Y.; Pu, H.; Wan, D., Polym. Chem. 2011, 2, 1287.
54. Villa, D. C.; Angioni, S.; Barco, S. D.; Mustarelli, P.; Quartarone, E., Adv. Energy
Mater. 2014, 4, 1301949.
55. Fang, J.; Lin, X.; Cai, D.; He, N.; Zhao, J., J. Membr. Sci. 2016, 502, 29.
56. He, C.; Han, K.-F.; Yu, J.-H.; Zhu, H.; Wang, Z.-M., Eur. Polym. J. 2016, 74, 168.
57. Maity, S.; Jana, T., Macromolecules 2013, 46, 6814.
58. Leroux, F. R.; Manteau, B.; Vors, J.-P.; Pazenok, S., Beilstein J. Org. Chem. 2008,
4, 13.
59. Lobato, J.; Cañizares, P.; Rodrigo, M. A.; Linares, J. J.; Pinar, F. J., Int. J.
Hydrogen Energy 2010, 35, 1347.
60. Seko, S.; Miyake, K.; Kawamura, N., J. Chem. Soc., Perkin Trans. 1 1999, 1437.
61. Navarrete-Vázquez, G.; Rojano-Vilchis, M. d. M.; Yépez-Mulia, L.; Meléndez, V.;
Gerena, L.; Hernández-Campos, A.; Castillo, R.; Hernández-Luis, F., Eur. J. Med.
Chem. 2006, 41, 135.
62. Ueda, M.; Sato, M.; Mochizuki, A., Macromolecules 1985, 18, 2723.
63. Yang, J. S.; Cleemann, L. N.; Steenberg, T.; Terkelsen, C.; Li, Q. F.; Jensen, J. O.;
Hjuler, H. A.; Bjerrum, N. J.; He, R. H., Fuel Cells 2014, 14, 7.

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