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研究生: 陳建忠
論文名稱: 以Ni-SDC作為固態氧化物燃料電池陽極材料行直接內部甲烷蒸氣重組反應之研究
Study of Ni-SDC anode for internal steam reforming of methane in solid oxide fuel cells
指導教授: 黃大仁
tj.huang
口試委員:
學位類別: 碩士
Master
系所名稱: 工學院 - 化學工程學系
Department of Chemical Engineering
論文出版年: 2003
畢業學年度: 91
語文別: 中文
中文關鍵詞: 固態氧化物燃料電池甲烷蒸氣重組
外文關鍵詞: sofc, steam reforming of methane
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  • 本研究以氧化釤添加氧化鈰(Samaria-doped Ceria)簡稱(SDC),
    混合硝酸鎳製成Ni-SDC作為固態氧化物燃料電池之陽極觸媒材料,在閉路的條件下,進行直接甲烷和直接甲烷內部蒸氣重組反應,並改變反應的溫度、陽極的燒結溫度及加入水氣的量,測量電池的電流,並以阻抗(impedance)分析法探討電池的阻力。

    實驗結果發現,電池的電流隨著反應溫度的升高而增加,應該是溫度愈高則電解質傳導氧離子的能力愈強,且反應的活性也是隨著溫度的上升而提昇。陽極燒結的溫度愈高,所表現出來的結果也愈好,可能是此時陽極的結構較緻密,陽極本身形成好的連結,進行電化學反應時能將電子快速的傳導出去,所以測得的電流較大,電池的反應阻力也較小。進行甲烷蒸氣重組反應時,在陽極上完全沒有積碳的生成,且電池都處在很穩定的狀態下,表示電池能夠長時間進行放電。

    另外,在實驗中也發現積碳有導電的功能,可作為陽極表面上金屬之間的橋樑;當金屬擔載量不足時,積碳不但能夠增加陽極的導電性,也因此能有效地傳導電子而促進電化學反應的發生,使電池電流增加。


    目錄…………………………………………………………………..…Ⅰ 圖目錄………………………………………………………………..…Ⅲ 表目錄…………………………………………………………………..VI 第一章 、緒論………………………………………………………….1 第二章 、文獻回顧……………………………………………………..7 2-1固態氧化物電解質……………………………………………….7 2-2 陰極材料………………………………………………………..11 2-3陽極電化學反應…………………………………………………12 2-4 陽極的微結構…………………………………………………..17 2-4.1 Ni的擔載量…………………………………………………17 2-4.2陽極的燒結溫度……………………………………………..18 第三章 、實驗方法與步驟……………………………………………20 3-1實驗藥品…………………………………………………………20 3-2實驗儀器…………………………………………………...……20 3-3陽極材料製備……………………………………………………21 3-4實驗裝置…………………………………………………………23 3-5電極材料的製備方法………………………….………………...24 3-6材料性質測試……………………………………………………24 3-7閉路電位的實驗步驟……………………………………………28 第四章 、結果與討論…………………………………………………30 4-1閉路電位下的實驗……………………………………………...30 4-2陽極的燒結溫度…………………………………………………39 4-2.1 Impedance分析法…………………………………………..39 4-3甲烷蒸氣重組反應………………………………………………42 4-4積碳對反應的影響………………………………………………48 4-5不同流速對還原的影響…………………………………………53 4-6通入氣體和不通入氣體的比較…………………………………55 4-7加水的影響…………………………………………………..…..57 第五章 、結論………………………………………..…………………60 第六章 、未來研究方向…………………………………………….…61 參考文獻………………………………………………………………..62

    1. Proceeding of fuel cell,COE/TPC/ITRI,1(1999)
    2 S.S.Penner,A.J,Appleby,etc, “Commercialization of Fuel Cells”,Progress in Energy and Combustion science,21,145-151(1995)
    3 M. Koyama, Ching-ju Wen, and Koichi Yamada, “La0.6Ba0.4CoO3 as a cathode material for solid oxide fuel cell using a BaCeO3 electrolyte”, J. Electrochem. Soc., 147, 87-91 (2000)
    4.A.Hammou and J.Guindet, “Solid Oxide Fuel Cell’’,in the CRC Handbook of Solid State Electrochemistry,P.T.Gellmgs and H.J.M.Bouwmeester,Eds.,CRC Pree.,407(1997)
    5.J.B.Goodenough, “Ceramic Solid Electrolytes’’,Solid State Ionic,94,17(1997)
    6. J.B.Goodenough, “Oxide-ion Conductors by design.’’, Nature
    ,404,821(2000)
    7 . H.Inaba,H.Tagawa, “Review Ceria-based Solid Electrolytes’,Solid State Ionics,83,1(1996)
    8.H.L.Tuller,in’’Nonstoichiometric’’.Academic Precc Inc Chap.6.(1981)
    9.P.J.Gellings,H.J.A.Koopmans and, A.J.Burggraff ,’’Electrocatalytic Phenomena in Gas Phase Reaction in Solid Electrolyte Electrochemical Cells’’,Appl.Catal,Vol.39,1(1988)
    10.P.J.Gellings and H.J.M.Bouemeester,“Ion and Mixed Conducting Oxides as Catalysts ”Catalysis Today,Vol.12,1(1991)
    11. S. J. Hong, K. Mehta, and A. V. Virkar, “Effect of Microstructure and Composition on Ionic-Conductivity of Rare-Earth Oxide-Doped Ceria”, J. Electrochem. Soc., 145, 638-647(1998)
    12. 鍾國濱博士論文, “以改良式溶膠-凝膠法製備氧化釤添加氧化鈰為固態氧化物燃料電池電解質材料及其電性研究”, 清華大學化工系,(2001)
    13.K.Mori.Hee Y.Lee,John B.Goodenough “Sr-and Ni-doped LaCoO3 and LaFeO3 perovskit:new cathode materials for solide-oxide fuel cells”,J.Electrochem Soc,145,3220(1998)
    14.Kim kinoshta, “Electrochemical Oxygen Techenology”,John Wiley&Sons.New York,1992,Chap.2&Chap.4
    15.O.Yamamoto,Y.Takeda,R.Kanno and M.Noda,’’Perovskite-type Oxides as Oxygen Electrodes for High Temperature Solid Oxide Fuel Cells’’,Solid State Ionics,22,241(1987)
    16. E. Hafel and H.G. Lintz,’’Elektrodencharakterisierumg und Grenzteperatur Beider Elektrochemischen Messungder SauerstoFFaktivitat an Platin’’, Solid State Ionics, 23,235-259(1987)
    17. B. A. van Hassel, B. A. Boukamp, and A. J. Burggraaf, “Electrode
    Polarization at Au,O2(g)/Yttria Stabilized Zirconia Interface.PartI: Theoretical Considerations of Reaction Model”,Solid State Ionics, 48, 139-154(1991)
    18. J. Mizusaki, H. Tagawa, Y. Miyaki, S. yamauchi and K. Hirano, “Knetics of The Electrode Reaction at The CO-CO2, Porous Pt/Stabilized Zirconia Interface ”,Solid State Ionics, 53, 126-134(1992)
    19. J. Mizusaki, K. Amano, S. yamauchi and K. Fueki, “Electrode Reaction at Pt,O2(g)/Stabilized Zirconia Interface .PartI: Theoretical Considerations of Reaction Model ”,Solid State Ionics, 22, 313-322(1987)
    20. J.Mizusaki, H.Tagawa and T.Saito, ”Preparation of Nickel Pattern Electrodes on YSZ and Their Electrochemical Properties in H2-H2O Atmospheres”,J. Electrochem. Soc., 141, 2129-2135 (1994)
    21.M.J.Saeki,H.Uchida and M.Watanbe,Catal Lett.,vol 26,149(1994)
    22. M.Watanade, H.Uchida, M.Shibata, N.Mochizuki and K.Amikura, “High Performance Catalyzed-Reaction Layer for Medium Temperature Operating Solid Oxide Fuel Cells”,J. Electrochem. Soc., 141,342-346(1994)
    23. K. Kendall*,C.M.finnerty,G.Saunder,J.t.Chung, “Effect of dilution on methane entering an SOFC anode”,J. Power Sources,106,323-327(2002)
    24. Jun Akikusa.aKazunori Adachi,aKoji Hoshino,aTatsumi I shihara,b.*and Yusaku Takitab, “Development of a Low Temperature Operation Solid Oxide Fuel Cell”, J. Electrochem. Soc.,148,1275-1278(2001)
    25 S. Ohara, R. Maric, X. Zhang, K. Mukai, T. Fukui, H. Yoshida, T. Inagaki, K. Miura, ”High performance electrodes for reduced temperatire solid oxide fuel cells with doped lanthanum gallate electrolyte I. Ni-SDC cermet anode”, J. Power Sources 86,455-458(2000)
    26.詹駿卿碩士論文,“以Ni-SDC作為直接甲烷固態氧化物燃料電池 極觸媒材料之研究”, 清華大學化工系,(2002)
    27. Takehisa Fukuia,*,Satoshi Oharaa,Makio Naitoa,Kiyoshi Nogib, “Performance and stabiltily of SOFC anode fabricated from NiO-YSZ composite particles”, J. Power Sources,110,91-95 (2002)
    28.B.Zhu*,”Advantage of intermediate temperature solid oxide fuel cells for tractionary applications’’,Journal of Power Sources,93,82-86(2001)
    29.B.C.H.Steele,in”High Comductivity Solid Ionic Conductor’’.ed.T.Takahashi(1989)
    30.Joon-Ho Koh,Young-Too*,Jin-Woo Parl,Hee Chun Lim,’’Carbon Deposition and Cell Performance Of Ni-YSZ Anode Suppoer Sofc With Methane Fuel’’,Solid State Ionics,149,157-166(2002)
    31.M.Brown,S.Primdahl,M.Mogensen,’’Structure/Performance Relationa for Ni/Yttria-Stabilized Zirconia Anodes for Solid Oxide Fuel Cells’’,J Electrochem.Soc.145,475(2000)
    32.M.Mogensen,S.Prinmdahl,J.T.Rheinlander,Proceedings of fourth internation Symposium on Solid Oxide Fuel Cells ,Electrochemical Society,Pennington NJ.659(1995)
    33.M.Mogensen,S.Skaarup,’’Kinetic and Geometric Aspects of Solid Oxide Fuel Cells’’, Solid State Ionics,86-88,1151(1996)
    34.Castro Luna,A.E.Becerra,A.M,’’Kinetics of Methane Steam Reforming on A Ni on Alumina-titania Catalyst’’.Reaction Kinetics&Catalysis Letters,61,369-374(1997)
    35.V.A.Sobyanin,V.D.Belyaev,T.I,Politova,O.A.Marina,’’Internal Steam Reforming of Methane over Ni-based Electrode in Solid Oxide Fuel Cells’’,Applied Catalysts(A:General),133,47(1995)
    36.P.Vernoux,M.Guillodo*,J.Fouletier,A.Hammou,’’Alternative Anode Material for Gradual Methane Reforming in Solid Oxide Fuel Cells’’,Solid State Ionics,135,425-431(2000)
    37.E.Perry Murray,T.Tsai & S.A.Barnett,’’A Direct-methane Fuell Cell With A Ceria-based Anode’’,Nature,400,august(1999)
    38..M.J Saeki,H.Uchida and M.Shibata,N.Mochizuki and K.Amikura,’’High Performance Catalyzed-Reaction Layer for Medium Teperature Operation Solid Oxide Fuel Cells ’’.J.Elcetrochem.Soc.141,342-345(1994)
    39.S.Mclntosh,J.M.Vohs*,and R.J.Gorte*,z,’’Role of Hydrocarbon Deposit in the Enhanced Performance of Dorect-Oxidation SOFCs’’,J.Electrochem.Soc.150,A470-A476(2003)
    40.H.Kim,C.LnW.L.Worrell,J.M.Vohs,and R.J.Gorte,’’Cu-Ni Cermet Anodes for Direct Oxidation of Methane in Solid-Oxide Fuel Cells’’,J.Electrochem.Soc.149,A247-A250(2002)

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