國立臺灣師範大學博碩士論文全文系統

簡易檢索 / 詳目顯示

回結果列表

研究生：	簡明芳 CHIEN MING FANG
論文名稱：	碳黑前處理對PtRu/C催化表現的影響 Effects of pretreatment of carbon black on PtRu/C catalysts performance
指導教授：	洪偉修 Hung, Wei-Hsiu
學位類別：	碩士 Master
系所名稱：	化學系 Department of Chemistry
論文出版年：	2008
畢業學年度：	96
語文別：	中文
論文頁數：	61
中文關鍵詞：	碳黑修飾、鉑釕催化劑、直接甲醇燃料電池
英文關鍵詞：	carbon black, PtRu catalyst, DMFC
論文種類：	學術論文
相關次數：	點閱：242 下載：0
分享至:	分享至facebook 分享至twitter

查詢本校圖書館目錄查詢臺灣博碩士論文知識加值系統勘誤回報

上一筆

在本研究，對直接甲醇燃料電池之陽極催化劑支持物(碳黑)進行化學處理，並測試其對甲醇電氧化的催化活性。碳黑經由過錳酸鉀、過錳酸鉀加硝酸、硝酸以及過氧化氫處理而官能基化。利用FT-IR和XPS來測定碳黑上表面含氧官能基。從結果發現，碳黑經由這些氧化處理可以讓表面含氧官能基增加。
我們以兩種方式來合成出碳黑支持鉑釕催化劑：還原和吸附。並藉由XPS、ICP-AES、XRD和TEM來鑑定鉑釕催化劑被支持在未處理和已處理的碳黑上。結果發現經由還原方式座落在碳黑之鉑釕的數量與碳黑表面含氧官能基的量有ㄧ定的相關性。碳黑表面的含氧官能基能增加表面上的可濕性，因而能讓前驅物更容易還原於碳黑表面上。利用對甲醇的CV和EIS實驗來測定催化劑的電催化活性。由結果知道，來自於經過官能基化的碳黑上之鉑釕的電催化性具有更好表現度，其中特別是經過過氧化氫修飾的碳黑。

The chemical treatment of the carbon black support on the performance for methanol electrooxidation was studied. The carbon black was functionalized with KMnO4, KMnO4+HNO3, HNO3 and H2O2. The surface oxygen complexes of the carbon black were determined with FT-IR and XPS. The results showed that the surface oxygen complexes of the carbon black increase after the oxidation treatments.
The PtRu catalysts were deposited on the carbon black with two different methods: reduction and adsorption. PtRu catalysts supported on the untreated and treated carbon blacks were characterized with XPS, ICP-AES, XRD, and TEM. The loading of the PtRu by reduction was related to the amount of surface oxygen complexes on the carbon black. The presence of surface oxygen complexes improves the wettability of the carbon black and, hence make the reduction of the precursors easier. The electrocatalytic activities of PtRu on the pretreated carbon black were investigated with the CV and EIS measurements in the oxidation of methanol. The pretreatment of carbon black, especially with H2O2, significantly improves the electrocatalytic performance.

謝誌 ----------------------------------------------------- I
中文摘要 ------------------------------------------------- II
英文摘要 ------------------------------------------------ III
第一章 序論 ----------------------------------------------- 1
    1-1 前言 --------------------------------------------- 1
    1-2 催化金屬對甲醇氧化的機制 ---------------------------- 2
    1-3 Pt與Ru原子比例對催化效果的影響 ---------------------- 5
    1-4 作為催化劑支持物的碳材修飾 -------------------------- 6
    1-5 催化劑製備法 -------------------------------------- 8
        1-5-1 含浸法(impregnation method) ---------------- 8
        1-5-2 微乳化法(microemulsion method) ------------- 8
        1-5-3 膠體法(colloidal method) ------------------- 9
        1-5-4 多醇法(polyol method) ---------------------- 9
        1-5-5 葡萄醣還原法(glucose reducetion processs) --- 9
第二章 原理 ---------------------------------------------- 10
    2-1 金屬前驅物的還原劑-乙二醇 -------------------------- 10
    2-2 分析儀器應用理論 ---------------------------------- 10
        2-2-1 傅立葉轉換紅外光譜儀(FT-IR) ----------------- 10
        2-2-2 誘導耦合電漿原子發射光譜(ICP-AES) ------------ 11
        2-2-3 粉末X光繞射儀(XRD) ------------------------- 12
        2-2-4 掃瞄式電子顯微鏡(SEM) ----------------------- 13
        2-2-5 穿透式電子顯微鏡(TEM) ----------------------- 14
        2-2-6  X-光光電子光譜分析儀(XPS) ------------------ 15
        2-2-7 循環伏安法(CV) ----------------------------- 17
        2-2-8 電化學阻抗譜(EIS) -------------------------- 19
第三章 實驗 ---------------------------------------------- 21
    3-1 實驗藥品 ----------------------------------------- 21
    3-2 碳黑前處理 --------------------------------------- 23
        3-3-1 將PtRu還原於碳黑上 ------------------------- 24
        3-3-2 將PtRu吸附於碳黑上 ------------------------- 25
    3-4 工作電極的製備 ----------------------------------- 25
    3-5 電性測試 ----------------------------------------- 26
第四章 結果與討論 ----------------------------------------- 27
    4-1 經過前處理之碳黑 ---------------------------------- 27
        4-1-1 經過前處理之碳黑的FT-IR鑑定 ----------------- 27
        4-1-2 經過前處理之碳黑的XPS鑑定 ------------------- 28
    4-2 將PtRu座落於碳黑上 ------------------------------- 32
      第一部份：將PtRu還原於碳黑上 ------------------------- 32
        4-2-1-1 PtRu＠C之XRD鑑定 ------------------------- 32
        4-2-1-2 PtRu＠C之TEM鑑定 ------------------------- 34
        4-2-1-3 PtRu＠C之ICP-AES鑑定 --------------------- 37
        4-2-1-4 PtRu＠C之XPS鑑定 ------------------------- 38
        4-2-1-6 PtRu＠C之催化效果測量 --------------------- 42
      第二部分：將PtRu吸附於碳黑上 ------------------------- 46
        4-2-2-1 PtRu＠C之XRD鑑定 ------------------------- 46
        4-2-2-2 PtRu＠C之SEM鑑定 ------------------------- 47
        4-2-2-3 PtRu＠C之TEM鑑定 ------------------------- 49
        4-2-2-4 PtRu＠C之ICP-AES鑑定 --------------------- 49
        4-2-2-5 PtRu＠C之XPS鑑定 ------------------------- 51
        4-2-2-6 PtRu＠C之催化效果測量 --------------------- 53
    4-3 結論 -------------------------------------------- 58
第五章 參考文獻 ------------------------------------------- 60
                                

(1) Hsin, Y. L.; Hwang, K. C.; Yeh, C. T. Journal of the American Chemical Society 2007, 129, 9999-10010.
(2) Barragan, V. M.; Heinzel, A. Journal of Power Sources 2002, 104, 66-72.
(3) Yang, C. W.; Wang, D. L.; Hu, X. G.; Dai, C. S.; Zhang, L. Journal of Alloys and Compounds 2008, 448, 109-115.
(4) Rao, V.; Simonov, P. A.; Savinova, E. R.; Plaksin, G. V.; Cherepanova, S. V.; Kryukova, G. N.; Stimming, U. Journal of Power Sources 2005, 145, 178-187.
(5) de la Fuente, J. L. G.; Martinez-Huerta, M. V.; Rojas, S.; Terreros, P.; Fierro, J. L. G.; Pena, M. A. Catalysis Today 2006, 116, 422-432.
(6) Iwasita, T.; Hoster, H.; John-Anacker, A.; Lin, W. F.; Vielstich, W. Langmuir 2000, 16, 522-529.
(7) Liu, H. S.; Song, C. J.; Zhang, L.; Zhang, J. J.; Wang, H. J.; Wilkinson, D. P. Journal of Power Sources 2006, 155, 95-110.
(8) Frelink, T.; Visscher, W.; Vanveen, J. A. R. Surface Science 1995, 335, 353-360.
(9) Hamnett, A. Catalysis Today 1997, 38, 445-457.
(10) Arbizzani, C.; Beninati, S.; Manferrari, E.; Soavi, F.; Mastragostino, M. Journal of Power Sources 2007, 172, 578-586.
(11) Yajima, T.; Uchida, H.; Watanabe, M. Journal of Physical Chemistry B 2004, 108, 2654-2659.
(12) Gasteiger, H. A.; Markovic, N.; Ross, P. N.; Cairns, E. J. Journal of Physical Chemistry 1994, 98, 617-625.
(13) Yasuda, K.; Nishimura, Y. Materials Chemistry and Physics 2003, 82, 921-928.
(14) Guo, J. W.; Zhao, T. S.; Prabhuram, J.; Chen, R.; Wong, C. W. Electrochimica Acta 2005, 51, 754-763.
(15) Lizcano-Valbuena, W. H.; Paganin, V. A.; Gonzalez, E. R. Electrochimica Acta 2002, 47, 3715-3722.
(16) Takasu, Y.; Fujiwara, T.; Murakami, Y.; Sasaki, K.; Oguri, M.; Asaki, T.; Sugimoto, W. Journal of the Electrochemical Society 2000, 147, 4421-4427.
(17) Hills, C. W.; Mack, N. H.; Nuzzo, R. G. Journal of Physical Chemistry B 2003, 107, 2626-2636.
(18) Dickinson, A. J.; Carrette, L. P. L.; Collins, J. A.; Friedrich, K. A.; Stimming, U. Electrochimica Acta 2002, 47, 3733-3739.
(19) Zhang, X.; Chan, K. Y. Chemistry of Materials 2003, 15, 451-459.
(20) Liu, Z. L.; Lee, J. Y.; Han, M.; Chen, W. X.; Gan, L. M. Journal of Materials Chemistry 2002, 12, 2453-2458.
(21) Liu, Y. C.; Qiu, X. P.; Chen, Z. G.; Zhu, W. T. Electrochemistry Communications 2002, 4, 550-553.
(22) Bock, C.; Paquet, C.; Couillard, M.; Botton, G. A.; MacDougall, B. R. Journal of the American Chemical Society 2004, 126, 8028-8037.
(23) Liu, J. C.; Qin, G. W.; Raveendran, P.; Kushima, Y. Chemistry-a European Journal 2006, 12, 2132-2138.
(24) Geng, D. S.; Chen, L.; Lu, G. X. Journal of Molecular Catalysis a-Chemical 2007, 265, 42-49.
(25) Skoog, D. A.; Holler, F. J.; Nieman, T. A. Principles of Instrumental Analysis; fifth ed.; Harcourt, 1998.
(26) 汪建民材料分析; 中國材料科學學會, 1998.
(27) Skoog, D. A.; West, D. M.; Holler, F. J.; Crouch, S. R. Fundamentals of Analytical Chemistry; 8th ed.; THOMSON, 2004.
(28) Bard, A. J.; Faulkner, L. R. ELECTOCHEMICAL METHODS Fundamentals and Applications; second ed.; John Wiley & Sons, Inc., 2001.
(29) Leng, Y. J.; Wang, X.; Hsing, I. M. Journal of Electroanalytical Chemistry 2002, 528, 145-152.
(30) Koczkur, K.; Yi, Q. F.; Chen, A. C. Advanced Materials 2007, 19, 2648-+.
(31) Pavia, D. L.; Lampman, G. M.; Kriz, G. S. Introduction to SPECTROSCOPY; third ed.; Thomson Learing, Inc. Thomson, 2001.
(32) Wang, Z. B.; Yin, G. P.; Shi, P. F. Carbon 2006, 44, 133-140.
(33) Yoon, H. G.; Kwon, K. W.; Nagata, K.; Takahashi, K. Carbon 2004, 42, 1877-1879.
(34) Moulder, J. F.; Stickle, W. F.; Sobol, P. E.; Bomben, K. D. Handbook of X-ray Photoelectron Spectroscopy; Perkin-Elmer Corporation Physical Electronics Division, 1992.
(35) Liu, Z. L.; Lee, J. Y.; Chen, W. X.; Han, M.; Gan, L. M. Langmuir 2004, 20, 181-187.
(36) Coloma, F.; Sepulvedaescribano, A.; Fierro, J. L. G.; Rodriguezreinoso, F. Langmuir 1994, 10, 750-755.
(37) Arico, A. S.; Antonucci, V.; Pino, L.; Antonucci, P. L.; Giordano, N. Carbon 1990, 28, 599-609.
(38) Camara, G. A.; Giz, M. J.; Paganin, V. A.; Ticianelli, E. A. Journal of Electroanalytical Chemistry 2002, 537, 21-29.
(39) Park, S. J.; Kim, K. D. Journal of Colloid and Interface Science 1999, 218, 331-334.

本全文未授權公開

簡易檢索 / 詳目顯示

相關論文