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研究生: 賴彥廷
論文名稱: 以(Ba0.5Sr0.5)0.9Sm0.1Co0.8Fe0.2O3-δ為SOFC陰極材料之研究
Study of (Ba0.5Sr0.5)0.9Sm0.1Co0.8Fe0.2O3-δ as SOFC Cathode Material
指導教授: 黃大仁
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: 2008
畢業學年度: 96
語文別: 中文
論文頁數: 67
中文關鍵詞: 固態氧化物燃料電池陰極材料BSSCCF一氧化氮還原
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  • 本研究以鈣鈦礦結構導氣離子材料(Ba0.5Sr0.5)0.9Sm0.1Co0.8Fe0.2O3-δ (BSSCF),搭配具有導氧離子性質的材料氧化釓參雜氧化鈰 (Ce0.9Gd0.1O2-x, Gadolinia doped Ceria,GDC )、對氮氧化物還原有催化助益的銅離子作為SOFC陰極材料,分別以氫氣、一氧化氮作為陰極氣體,進行電池性能、交流阻抗分析( AC Impedance ) 等電性分析,希望能藉此驗證以固態氧化物燃料電池處理一氧化氮是否可行。
    實驗發現以單純BSSCF為陰極材料於不同操作溫度下進行單電池發電,以20%氧氣為陰極氣體情況下,電池之maximum power density可達4.79 mW/cm2 (800℃)、6.09 mW/cm2 (850℃)、8.65 mW/cm2 (900℃)、11.33 mW/cm2 (950℃)。若將BSSCF與不同比例GDC混合,發現GDC添加量越多電池效能越佳,於800℃下操作,使用20%氧氣為陰極氣體時,BSSCF添加50wt%GDC為陰極材料之電池maximum power density 可達8.65 mW/cm2;以BSSCF 添加70wt%GDC為陰極材料則可達16.28 mW/cm2。若改用6%一氧化氮為陰極氣體,於800℃下操作時,BSSCF混合GDC為陰極材料效果相當差,BSSCF添加50wt%GDC maximum power density 僅有0.031mW/cm2;BSSCF 添加70wt%GDC僅有0.1017mW/cm2。若於BSSCF結構中添加銅離子構成BSSCCF 712[(Ba0.5Sr0.5)0.9Sm0.1Co0.7Cu0.1Fe0.2O3-δ] (銅離子取代鈷離子)、BSSCCF 811 [(Ba0.5Sr0.5)0.9Sm0.1Co0.8Cu0.1Fe0.1O3-δ] (銅離子取代鐵離子),則電池效能可以提升至0.8 mW/cm2 (BSSCCF 712)、1.66 mW/cm2(BSSCCF 811),顯示銅離子對於一氧化氮還原催化活性之提升有所助益。


    This Study used (Ba0.5Sr0.5)0.9Sm0.1Co0.8Fe0.2O3-δ (BSSCF) as major cathode material, combined with Gadolinia doped Ceria and copper ion for SOFC. For different cathode material, we provide 20% O2 and 6% NO from cathode side to conduct single cell SOFC test and try to show that NO can be used at cathode side of SOFC.
    Experiment shows that SOFC single cell with only BSSCF cathode under different temperature, applying 20% O2 from cathode side could provide maximum power density 4.79 mW/cm2 (800℃)、6.09 mW/cm2 (850℃)、8.65 mW/cm2 (900℃)、11.33 mW/cm2 (950℃).
    Combined BSSCF with different wt% of Gadolinia Doped Ceria (GDC) can found that the more wt% GDC added, the better SOFC single performance provided. BSSCF with 50wt%GDC as cathode could provide maximum power density 8.65 mW/cm2, while BSSCF with 70wt%GDC could reach 16.28 mW/cm2, under 800℃ with 20% O2 applied from cathode side.
    When applying 6% NO from cathode side, BSSCF with GDC could only provide limited performance. If we added Copper into BSSCF perovskite structure to form BSSCCF 712 or BSSCCF 811, cell performance could raise remarkably. Maximum power density can reach 0.8 mW/cm2 (BSSCCF 712), and 1.66 mW/cm2(BSSCCF811), showing that copper ion is really helpful for NO redution.

    第一章 緒論 1 第二章 文獻回顧 3 2-1 燃料電池簡介 3 2-2 固態氧化物燃料電池 5 2-2-1 固態氧化物燃料電池發電原理 6 2-2-2 固態氧化物燃料電池之極化 7 2-3 固態氧化物燃料電池電解質材料 9 2-4 固態氧化物燃料電池陽極材料 11 2-5 固態氧化物燃料電池陰極材料 11 2-5-1 鈣鈦礦結構( Perovskite Structure ) 13 2-5-2 鈣鈦礦結構陰極材料 15 2-6 電化學方法處理氮氧化物 17 第三章 研究規劃 19 第四章 實驗方法與步驟 21 4-1 實驗藥品/氣體 21 4-2 製備方法 22 4-2-1 (Ba0.5Sr0.5)0.9Sm0.1Co0.8Fe0.2O3-δ (BSSCF) 22 4-2-2 (Ba0.5Sr0.5)0.9Sm0.1Co0.7Cu0.1Fe0.2O3-δ (BSSCCF 712) 22 4-2-3 (Ba0.5Sr0.5)0.9Sm0.1Co0.8Cu0.1Fe0.1O3-δ (BSSCCF 811) 23 4-2-4 氧化釓參雜氧化鈰 (Ce0.9Gd0.1O2-x , Gadolinia doped Ceria) 24 4-2-5 BSSCF/GDC、BSSCCF712/GDC、BSSCCF811/GDC系統 24 4-3 實驗儀器 25 4-4 實驗方法 28 4-4-1 氫氣程溫還原反應(H2-TPR) 28 4-4-2 二氧化碳程溫氧化反應(CO2-TPO) 28 4-4-3 電池單元製備 29 4-4-4 電池性能測試 30 4-4-5 交流阻抗分析(AC Impedance) 30 第五章 結果與討論 33 5-1 X光繞射(XRD, X-Ray Diffraction) 33 5-1-1 BSSCF 33 5-1-2 BSSCCF712、BSSCCF811 34 5-1-3 GDC 34 5-2 掃描式電子顯微鏡(SEM, Scanning Electron Microscopy) 36 5-3 氫氣程溫還原反應(H2-TPR,) 37 5-4 二氧化碳程溫氧化反應(CO2-TPO) 39 5-5 電池效能 41 5-5-1 BSSCF 41 5-5-2 BSSCF with 50wt% GDC & BSSCCF with 70wt% GDC 43 5-5-3 BSSCCF811 & BSSCCF712 47 5-6 AC Impedance 52 第六章 結論 60 第七章 未來展望 61 第八章 參考文獻 63

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