Title page for 942203023


[Back to Results | New Search]

Student Number 942203023
Author Che-hsun Pai(白哲勳)
Author's Email Address No Public.
Statistics This thesis had been viewed 1942 times. Download 1043 times.
Department Chemistry
Year 2006
Semester 2
Degree Master
Type of Document Master's Thesis
Language zh-TW.Big5 Chinese
Title Proton Transport Properties of Acid-Base Polyelectrolyte
Date of Defense 2007-06-28
Page Count 74
Keyword
  • acid-base polyelectrolyte
  • proton transport
  • Abstract ABPBI is synthesized successfully in this research. After synthesized , ABPBI mix with three different acid polymers PVSA, PVPA, and PAA to form acid-base polyelectrolyte membranes. FT-IR and XRD data show that the compatibility between acid and base polymers is high because of the acid-base interaction, Besides, after adding small amount of acid polymer in ABPBI, the regular arrangement of ABPBI is destroyed because of the acid-base interaction. The interaction between ABPBI and PVSA is the strongest of all the membranes, even the 50ABPBI-50PVSA is similar to the formation of salt. All the membranes have high thermal stability up to 200℃, it means that the membranes can be used safely in high temperature fuel cells. If acid and base polymers mix well to form an ordered structure, the decomposition temperature of functional groups is increasing, and the thermal stability is higher.
      Variable temperature conductivity for dry membranes follows the Arrhenius law. With the increase of temperature, the proton conductivity is increasing. In ABPBI-PVPA system, 50:50 ratio shows the lowest proton conductivity. High resolution solid state NMR shows that ABPBI and PVPA form a compact complex when the ratio is 50:50. This result suggests that the proton is more easily to transport in this membrane. In the wet condition, proton conductivity increase with increasing temperature before water loss temperature. When water starts to vaporize, proton conductivity drops quickly, it means water is the major medium to transport proton in membranes. According to the data above, the hopping and vehicle mechanism to transport proton both exist in membranes, and ABPBI-PVPA system shows the highest proton conductivity in dry and wet conditions. It means the interaction between imidazole and phosphonic acid is suitable for proton transport.
    Table of Content 中文摘要…………………………………………………………………i
    英文摘要………………………………………………………………iii
    謝誌……………………………………………………………………iv
    目錄………………………………………………………………………v
    表目錄………………………………………………………………viii
    圖目錄………………………………………………………………ix
    第一章 緒論
    1-1前言…………………………………………………………1
    1-2研究動機……………………………………………………2
    第二章 高溫電解質薄膜文獻回顧
    2-1 Nafion®薄膜的修飾
    2-1-1 使用非純水溶劑…………………………………......6
    2-1-2 添加親水性氧化物或固態無機物………………......7
    2-2使用碳氫化合物高分子取代Nafion®……………………...11
    2-3 有機/無機複合物薄膜……………………………………..14
    2-4 酸/鹼高分子薄膜
    2-4-1 鹼性高分子/酸性小分子…………………………...21
    2-4-2 鹼性小分子/酸性高分子…………………………...24
    2-4-3 鹼性高分子/酸性高分子…………………………...25
    第三章 實驗操作
    3-1 樣品製備與實驗步驟
    3-1-1 ABPBI之合成…………………………………….....29
    3-1-2 電解質薄膜之製備…………………………………29
    3-1-3 實驗步驟……………………………………………30
    3-2 實驗藥品…………………………………………………...31
    第四章 結果與討論
    4-1 ABPBI之鑑定
    4-1-1 13C固態核磁共振儀( 13C Solid State NMR )………….....32
    4-1-2 傅立葉紅外線光譜儀(FT-IR)分析……………………...32
    4-1-3 X光繞射儀(XRD)分析…………………………………...33
    4-1-4 熱重損失分析儀(TGA)……………………………….....36
    4-2 酸鹼混合高分子電解質薄膜結構分析
    4-2-1 傅立葉紅外線光譜儀(FT-IR)分析……………………...38
    4-2-2 X光繞射儀(XRD)分析…………………………………...41
    4-2-3 熱重分析儀(TGA)分析……………………………….....45
    4-2-4 微差掃瞄熱卡計(DSC)分析………………………….....49
    4-3 酸鹼混合高分子電解質薄膜質子傳遞行為分析
    4-3-1 無水條件下質子傳遞行為……………………………....52
    4-3-2 含水條件下質子傳遞行為………………………………60
    第五章 結論與未來展望………………………………………………...66
    第六章 參考文獻………………………………………………………...69
    Reference 1. Li, Q.; He, R.; Gao, J.; Jensen, J. O.; Bjerrum, N. J. J. Electrochem. Soc. 2003, 150, A1599.
    2. G. Pourcelly ; A. Oikonomou ; H.D. Hurwitz ; C. Gavach, J. Electroanal. Chem. 1990, 287, 43.
    3. Ronghuan He ; Qingfeng Li ; Gang Xiao ; Niels J. Bjerrum, Journal of Membrane Science 2003, 226, 169.
    4. Qingfeng Li ; Ronghuan He ; Rolf W. Berg ; Hans A. Hjuler ; Niels J. Bjerrum, Solid State Ionics 2004, 168, 177.
    5. Palanichamy Krishnan ; Jin-Soo Park ; Chang-Soo Kim, Journal of Power Sources 2006, 159, 817.
    6. S. R. Narayanan ; Shiao-Pin Yen ; L. Liu ; S. G. Greenbaum, J. Phys. Chem. B 2006, 110, 3942.
    7. Florjanczyk, Z.; Wielgus-Barry, E.; Poltarzewski, Z. Solid State Ionics 2001, 145,119.
    8. Savinell, R.; Yeager, E.; Tryk, D.; Landau, U.; Wainright, J.; Weng, D.; Lux, K.;Litt, M.; Rogers, C. J. Electrochem. Soc. 1994, 141, L46
    9. Malhotra, S.; Datta, R. J. Electrochem. Soc. 1997, 144, L23.
    10. Doyle, M.; Choi, S. K.; Proulx, G. J. Electrochem. Soc. 2000, 147, 34.
    11. Sun, J.; Jordan, L. R.; Forsyth, M.; MacFarlane, D. R. Electrochim. Acta 2001, 46, 1703.
    12. Watanabe, M.; Uchida, H.; Seki, Y.; Emori, M. The Electrochemical Society Meeting; PV94-2, Abstract No. 606; Electrochemical Society: Pennington, NJ, 1994, 946
    13. Mauritz, K. A. Mater. Sci. Eng., C 6, 1998, 121.
    14. Miyake, N.;Wainwright, J.S.;Savinell, R.F. J. Electrochem. Soc. 2001, 148, A898.
    15. Zoppi, R. A.; Yoshida, I. V. P.; Nunes, S. P. Polymer 1997, 39,1309.
    16. Zoppi, R. A.; Nunes, S. P. J. Electroanal. Chem. 1997, 445, 39.
    17. K. T. Adjemian ; S. J. Lee ; S. Srinivasan ; J. Benziger ; A. B. Bocarsly Journal of The Electrochemical Society 2002, 149, A256.
    18. Antonucci, P. L.; Arico´, A. S.; Creti, P.; Ramunni, E.; Antonucci,V. Solid State Ionics 1999, 125, 431.
    19. Yang, C.; Srinivasan, S.; Arico`, A. S.; Creti, P.; Baglio, V.; Antonucci, V. Electrochem. Solid-State Lett. 2001, 4, A31.
    20. Adjemian, K.T.;Lee, S.J.;Srinivasan, S.;Benziger, J;Bocarsly, A.B. J. Electrochem. Soc. 2002, 149, A256.
    21. Staiti, P.; Arico, A. S.; Baglio, V.; Lufrano, F.; Passalacqua, E.;Antonucci, V. Solid State Ionics 2001, 145, 101.
    22. K.T. Adjemian ; S.J. Lee ; S. Srinivasan, J. Benziger ; A.B. Bocarly, J. Electrochem. Soc. 2002, 149, A256.
    23. Z.G. Shao ; H. Xu ; M. Li ; I.-M. Hsing, Solid State Ionics 2006, 177, 779.
    24. P. Costamagna ; C. Yang ; A.B. Bocarsly ; S. Srinivasan, Electrochim. Acta 2002, 47, 1023.
    25. C. Yang ; S. Srinivasan ; A.B. Bocarsly ; S. Tulyani ; J.B. Benziger, J. Membr. Sci. 2004, 237, 145.
    26. V. Ramani ; H.R. Kunz ; J.M. Fenton ; J. Membr. Sci. 2004, 232, 31.
    27. V. Ramani ; H.R. Kunz ; J.M. Fenton ; Electrochim. Acta 2004, 50, 1181.
    28. S.H. Kwak ; T.H. Yang ; C.S. Kim ; K.H.Yoon, Electrochim. Acta 2004, 50, 653.
    29. S.H. Kwak ; T.H. Yang ; C.S. Kim ; K.H.Yoon, Solid State Ionics 2003, 160, 309.
    30. Y. Si ; H.R. Kunz ; J.M. Fenton, J. Electrochem. Soc. 2004, 151, 623.
    31. Y.F. Zhai ; H.M. Zhang ; J.W. Hu ; B.L. Yi, J. Membr. Sci. 2006, 280, 148.
    32. Kawahara, M. ; Rikukawa, M. ; Sanui, K. ; Ogata, N. Solid State Ionics 2000, 136-137, 1193.
    33. Kawahara, M. ; Rikukawa, M. ; Sanui, K. Polym. Adv. Technol. 2000, 11, 544.
    34. Asensio, J.A. ; Borros, S. ; Gomez ,Romero, J. Polym. Sci. Part A :Polym. Chem. 2002, 40, 3703.
    35. Kobayashi T ; Rikukawa M ; Sanui K ; Ogata N., Solid State Ionics 1998, 106, 219.
    36. Bishop MT ; Karasz FE ; Russo PS ; Langley KH., Macromolecules 1985, 18 ,86.
    37. Devaux J ; Delimoy D ; Daoust D ; Legras R ; Mercier JP ; Strazielle C ; Neild E., Polymer 1985, 26, 1994.
    38. Nolte, R.; Ledjeff, K.; Bauer, M.; Muぴ lhaupt, R. J. Membr. Sci. 1993, 83, 211.
    39. Kerres, J.; Zhang, W.; Cui, W. J. Polym. Sci. Part A 1998, 36, 1441
    40. Kerres, L.; Cui, W.; Junginger, M. J. Membr. Sci. 1998, 139, 227.
    41. Kerres, J. A. J. Membr. Sci. 2001, 185, 3.
    42. Genies, C.; Mercier, R.; Sillinon, B.; Cornet, N.; Gebel, G.; Pineri, M., Polymer 2001, 42, 359.
    43. Vallejo, E.; Gavach, C.; Pineri, M. J. Power Sources 1999, 160, 127.
    44. Guo, X.; Fang, J.; Watari, T.; Tanaka, K.; Kita, H.; Okamoto, Macromolecules 2002, 35, 6707.
    45. Child, A. D.; Reynolds, J. R. Macromolecules 1994, 27, 1975.
    46.. Rulkens, R.; Schulze, M. Macromol. Rapid Commun. 1994, 15, 669.
    47. Miyatake, K.; Iyotani, H.; Yamamoto, K.; Tscuchida, E. Macromolecules 1996, 29, 6969.
    48. Hruszka, P.; Jurga, J.; Brycki, B. Polymer 1992, 33, 248.
    49. Kosmala, B.; Schauer, J. J. Appl. Polym. Sci. 2002, 85, 1118.
    50. Miyatake, K.; Shouji, E.; Yamamoto, K.; Tsuchida, E. Macromolecules 1997, 30, 2941.
    51. Kopitzke, R. W.; Linkous, C. A.; Nelson, G. L. J. Polym. Sci. 1998, 36, 1197.
    52. Guo, Q.; Pintauro, P. N.; Tang, H.; O’Connor, S. J. Polym. Sci. 1999, 154, 175.
    53. Staiti, P.; Minutoli, M.; Hocevar, S. J. Power Sources 2000, 90, 231.
    54. Staiti, P.; Minutoli, M. J. Power Sources 2001, 94, 9
    55. Nakajima, H.; Honma, I. Solid State Ionics 2002, 148, 607.
    56. Honma, I.; Nomura, S.; Nakajima, H. J. Membr. Sci. 2001, 185, 83.
    57. Nakajima, H.; Nomura, S.; Sugimoto, T.; Nishikawa, S.; Honma, I, J. Electrochem. Soc. 2002, 149, A953.
    58. Amarilla, J. M.; Rojas, R. M.; Rojo, J. M.; Cubillo, M. J.; Linares,A.; Acosta, J. L. Solid State Ionics 2000, 127, 133.
    59. Bonnet, B.; Jones, D. J.; Roziere, J.; Tchicaya, L.; Alberti, G.; Casciola, M. Massinelli, L.; Baner, B.; Peraio, A.; Ramunni, E. J. New Mater. Electrochem. Syst. 2000, 3, 87.
    60. Zaidi, S. M. J. Mikhailenko, S. D.; Robertson, G. P.; Guiver, M. D.; Kaliaguine, S. J. Membr. Sci. 2000, 173, 17.
    61. Nunes, S. P.; Ruffmann, B.; Rikowski, E.; Vetter, S.; Richau, K. J. Membr. Sci. 2002, 203, 215.
    62. Mikhailenko, S. D.; Zaidi, S. M. J.; Kaliaguine, S. Catal. Today, 2001, 67, 225.
    63. Rozie´re, J.; Jones, D. J.; Tchicaya-Bouckary, L.; Bauer, B. WO 02/05370, 2000.
    64. Genova-Dimitrova, P.; Baradie, B.; Foscallo, D.; Poinsignon, C.; Sanchez, J. Y. J. Membr. Sci. 2001, 185, 59.
    65. Baradie, B.; Poinsignon, C.; Sanchez, J. Y.; Piffard, Y.; Vitter, G.; Bestaoui, N.; Foscallo, D.; Denoyelle, A.; Delabouglise, D.; Vaujany, M. J. Power Sources 1998, 74, 8.
    66. Mauritz, K. A. Mater. Sci. Eng., C 1998, 6, 121.
    67. Malhotra, S.; Datta, R. J. Electrochem. Soc. 1997, 144, L23.
    68. Yang, C.; Srinivasan, S.; Arico`, A. S.; Creti, P.; Baglio, V.;Antonucci, V. Electrochem. Solid-State Lett. 2001, 4, A31.
    69. Alberti, G.; Casciola, M.; Palombari, R. J. Membr. Sci. 2000, 172, 233.
    70. Genova-Dimitrova, P.; Baradie, B.; Foscallo, D.; Poinsignon, C.; Sanchez, J. Y. J. Membr. Sci. 2001, 185, 59.
    71. Hickner, M.;Kim, Y.S.;Wang, F.;Zawodzinski, T.A.;McGrath, J.E. SAMPE Tech. Conf. 2001, 33, 1519.
    72. Staiti, P. J. New Mater. Electrochem. Syst. 2001, 4, 181.
    73. Itaru Honma, Hitoshi Nakajima and Shigeki Nomura Solid State Ionics 2002, 154– 155, 707.
    74. Honma, I.;Nomura, S.;Nakajima, H. J. Membr. Sci. 2001, 185, 83.
    75. Honma, I.;Nomura, S.;Sugimoto, T.;Nakajima, H. J. Electrochem. Soc. 2002, 149, A953.
    76. Masanori Yamada Itaru Honma J. Phys. Chem. B 2006, 110, 20486.
    77. Bonnet, B.; Jones, D. J.; Roziere, J.; Tchicaya, L.; Alberti, G.; Casciola, M. Massinelli, L.; Baner, B.; Peraio, A.; Ramunni, E. J. New Mater. Electrochem. Syst. 2000, 3, 87.
    78. Zaidi, S. M. J. Mikhailenko, S. D.; Robertson, G. P.; Guiver, M. D.; Kaliaguine, S. J. Membr. Sci. 2000, 173, 17.
    79. Mikhailenko, S. D.; Zaidi, S. M. J.; Kaliaguine, S. Catal. Today, 2001, 67, 225.
    80. Rozie´re, J.; Jones, D. J.; Tchicaya-Bouckary, L.; Bauer, B. WO 02/05370, 2000.
    81. Hickner, M.; Kim, Y. S.; Wang, F.; Zawodzinski, T. A.; McGrath,J. E. Proc. 33rd Int. SAMPE Techn. Conf. 2001, 33, 1519.
    82. Staiti, P.; Minutoli, M. J. Power Sources 2001, 94, 9.
    83. Staiti, P.; Minutoli, M.; Hocevar, S. J. Power Sources 2000, 90, 231.
    84. Boysen, D. A.; Chrisholm, C. R. I.; Haile, S. M.; Sekharipuram, V.; Narayanan, R. J. Electrochem. Soc. 2000, 147, 3610.
    85. Park, Y.; Nagai, M. Solid State Ionics 2001, 145, 149.
    86. Stangar, U. L.; Orel, B.; Groselj, N.; Judeinstein, P.; Decker, F.; Lianos, P. Monatsh. Chem. (Chem. Monthly) 2001, 132, 103.
    87. Honma, I.; Nakajima, H.; Nishikawa, O.; Sugimoto, T.; Nomura, S. J. Electrochem. Soc. 2002, 149, A1389.
    88. Lavrencic S. U.; Groselj, N.; Orel, B.; Schmitz, A.; Colomban, P. Solid State Ionics 2001, 145, 109.
    89. Honma, I.; Nomura, S.; Nakajima, H. J. Membr. Sci. 2001, 185, 83.
    90. Nakajima, H.; Nomura, S.; Sugimoto, T.; Nishikawa, S.; Honma, I, J. Electrochem. Soc. 2002, 149, A953.
    91. Vaivars, G.; Azens, A.; Grangvist, C. G. Solid State Ionics 1999, 119, 269.
    92. Park, Y.-I.; Dong, K. J.; Nagai, M. J. Mater. Sci. Lett. 2000, 19, 1735.
    93. Park, Y.-I.; Kim, J.-D.; Nagai, M. Materials Research Society Symposium Proceedings 2000, 600, 305.
    94. Donoso P. ; Gorecki W. ; Berthier C. ; Dfendini F. ; Poinsignon C. ; Armand MB. Solid State Ionics 1988, 28, 969.
    95. Senadeera GKR. ; Gareem MA. ; Skaarup S. ; West K. Solid State Ionics 1996, 85, 37.
    96. Gupta PN. ; Singh KP. Solid State Ionics 1996, 86, 319.
    97. Vargas MA. ; Vargas RA. ; Mellander B-E. Electrochim Acta 1999, 44, 4227.
    98. Bozkurt, A..; Meyer, W.H. Solid State Ionics 2001, 138, 259.
    99. Tsuruhara K. ; Rikukawa M. ; Sanui K. ; Ogata N. ; Nagasaki Y. ; Kato M. Electrochim Acta 2000, 45, 1391.
    100. Stevens JR ; Wieczorek W. ; Raducha D. ; Jeffrey KR. Solid State Ionics 1997, 97, 347.
    101. Wieczorek W. ; Stevens JR. Polymer 1997, 38, 2057.
    102. Qingfeng, L. ; Hjuler, H.A. ; Bjerrum, N.J. J. Appl. Electrochem. 2001, 31, 773.
    103. S. R. Narayanan ; Shiao-Pin Yen ; L. Liu ; S. G. Greenbaum J. Phys. Chem. B 2006, 110, 3942
    104. Hong-ting Pu ; Lei Qiao ; Qi-zhi Liu ; Zheng-long Yang European Polymer Journal 2005, 41, 2505.
    105. Masanori Yamada ; Itaru Honma Polymer 2005, 46, 2986.
    106. Liu Yifeng ; Yu Qinchun ; Yuan Jun ; Ma Liangliang ; Wu Yihua European Polymer Journal 2006, 42, 2199.
    107. Masanori Yamada ; Itaru Honma Polymer 2004, 45, 8349.
    108. Wonbong Jang ; Saimani Sundar ; Seunghyuk Choi ;Yong-Gun Shul ; Haksoo Han Journal of Membrane Science 2006, 280, 321.
    109. M. Luisa Di Vona ; Alessandra D’Epifanio ; Debora Marani ; Marcella  Trombetta ; Enrico Traversa ; Silvia Licoccia Journal of Membrane Science 2006, 279, 186
    110. Z S.M. Javaid Zaidi Electrochimica Acta 2005, 50, 4771.
    111. Jochen Kerres ; Andreas Ullrich ; Frank Meier ; Thomas Haring Solid State Ionics 1999, 125, 243.
    112. Bouchet, R.; Siebert, E. Solid State Ionics 1999, 118, 287.
    113. Colan E. Hughes ; Stefan Haufe ; Brigitta Angerstein ; Ratna Kalim ; Ulrich Ma1hr ; Annette Reiche ; Marc Baldus,J. Phys. Chem. B 2004, 108, 13626.
    114. Adjemian, K. T.; Srinivasan, S.; Benziger, J.; Bocarsly, A. B. J. Power Sources 2002, 109, 356.
    115. A.V. Anantaraman ; C.L. Gardner J. Electroanal. Chem. 1996, 414, 115.
    116. Costamagna, P.; Yang, C.; Bocarsly, A. B.; Srinivasan, S. Electrochim. Acta 2002, 47, 1023.
    117. Q.F. Li ; H.A. Hjuler ; N.J. Bjerrum J. Appl. Electrochem. 2001, 31, 773.
    118. J.T.Wang ; R.F. Savinell ; J.S.Wainright ; M. Litt, H.Yu Electrochim. Acta 1996, 41, 193.
    119. V. Deimede ; G.A. Voyiatzis ; J.K. Kallitsis ; L. Qingfeng ; N.J. Bjerrum Macromolecules 2000, 33, 7609.
    120. Q.F. Li ; H.A. Hjuler ; C. Hasiotis ; J.K. Kallitsis ; C.G. Kontoyanni ; N.J. Bjerrum Electrochem. Solid State Lett. 2002, 5, A125.
    121. C. Hasiotis ; L. Qingfeng ; V. Deimede ; J.K. Kallitsis ; C.G. Kontoyannis ; N. J. Bjerrum J. Electrochem. Soc. 2001, 148, A513.
    122. Jochen Meier-Haack ; Antje Taeger ; Claus Vogel ; Kornelia Schlenstedt ; Wolfgang Lenk Dieter Lehmann Separation and Purification Technology 2005, 41, 207.
    123. Donald L. Pavia ; Gary M, Lampman ; George S. Kriz , Introduction to Spectroscopy third edition, Brookscole, 2001.
    124. Pedro G´omez-Romero ; Juan Antonio Asensio ; Salvador Borr
    Advisor
  • Peter Po-jen Chu(諸柏仁)
  • Files
  • 942203023.pdf
  • approve immediately
    Date of Submission 2007-07-17

    [Back to Results | New Search]


    Browse | Search All Available ETDs

    If you have dissertation-related questions, please contact with the NCU library extension service section.
    Our service phone is (03)422-7151 Ext. 57407,E-mail is also welcomed.