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  • 學位論文

陽極支撐型固態氧化物燃料電池之電解質薄膜製程與分析

Processing and Characterization of Electrolyte Thin Filmfor Anode-Supported Solid Oxide Fuel Cell

指導教授 : 韋文誠

摘要


本研究採用兩種方法來製備釔安定化氧化鋯(YSZ)與釔摻雜氧化鈰(YDC)薄膜,用以改善陽極支撐型固態氧化物燃料電池的效率,包含溶膠鍍膜法(sol-state deposition)與膠粒鍍膜法(colloidal deposition)。使用這些方法製備的4-8 mol% 釔安定化氧化鋯薄膜可以達到無裂痕且緻密的要求,在600oC下測試,使用溶膠鍍膜法製備具有0.50 um的4 mol%釔安定化氧化鋯薄膜的單電池,其功率密度可達到477 mW/cm2,高於文獻報導具有數微米的8 mol%釔安定化氧化鋯薄膜的單電池;另外,使用膠體鍍膜法,單次鍍膜亦可成功製備出厚度2.5~8 um無裂痕的釔安定化氧化鋯(YSZ)薄膜。 為了避免釔安定化氧化鋯(YSZ)電解質與鑭鍶錳氧化物(LSM)陰極產生反應,本研究中,使用膠體鍍膜法製備釔摻雜氧化鈰(YDC)電解質薄膜層隔絕,並使用X光繞射儀(XRD)與高解析度穿透式電子顯微鏡(HRTEM)分析釔安定化氧化鋯(YSZ)與釔摻雜氧化鈰(YDC)材料的固溶反應現象,結果顯示反應溫度超過1200oC開始產生固溶反應,當反應溫度高於1600oC時達到完全固溶. 在1300oC時鈰離子擴散到氧化鋯的速度比鋯離子擴散到氧化鈰的速度快。 研究中針對製備單電池進行各項的電化學性質進行分析,包含開路電壓(OCV)、比表面積電阻(ASR)與單電池電效率(I-V-P)等。結果顯示,單電池組的功率可以藉由各項改良來提升,包含電流收集板(current collector)與陰極的接觸、陰極端鎳基多孔電流收集板的氧化、鑭鍶鈷鐵氧化物(LSCF)取代鑭鍶錳氧化物(LSM)陰極與使用新的層狀結構等。

並列摘要


Various thin yttria-stabilized zirconia (YSZ) and ceria (YDC) electrolytic films on anode-supported solid oxide fuel cell (SOFC) have been prepared to improve the performance of the made cells by either a sol-state deposition or colloidal deposition (CD) process. 4-8 mol% yttria-doped zirconia layer was prepared to reach the requirements of crack-free, dense and thin coats. The best half cell consisted of 4YSZ film with 0.5 um thickness showed a higher power density (477 mW/cm2) at 600oC than the cell with microns 8YSZ electrolyte layer. The CD method is also able to prepare crack-free and dense YSZ films in thickness of 2.5~8 um on porous anode substrate via one coating cycle. YDC as the second electrolytic layer is prepared by colloidal deposition to prevent the reaction of YSZ/(La,Sr)MnOx (LSM). The solid solution reaction between YSZ and YDC has been analyzed. XRD and high resolution TEM results show that the reaction of YSZ and YDC layers starts at 1200oC, and becomes fully solid solution at 1600oC. The diffusion of Ce ions into YSZ grains is faster than the reversed migration of Zr ions into YDC at 1300oC. Electrochemical analysis on assembled cells has been conducted. By measuring the open circuit voltage (OCV), area specific resistance (ASR), and current-voltage-power (I-V-P), the power density of made gas-tight cells can be improved step-by-step in consideration of the interface contact between current collector/cathodes, oxidation of Ni-foam at cathode in oxidation condition, the replacement of LSM by LSCF cathode material, and new arrangement of layer configuration.

並列關鍵字

electrolyte YSZ SOFC Power density solid solution

參考文獻


[1] National Hydrogen Energy Roadmap, issued by U.S. Department of Energy, 2002.
[3] G. J. K. Acres, “Recent advances in fuel cell technology and its applications,” J. Power Sources, 100, 60-66 (2001).
[4] G. C. Kostogloudis, G. Tsiniarakis, C. Ftikos, “Chemical reactivity of perovskite oxide SOFC cathodes and yttria stabilized zirconia,” Solid State Ionics, 135, 529-535 (2000).
[5] H. Mitsuyasu, Y. Nonaka, K. Eguchi, and H. Arai, “TEM Observation of Reaction at the Interface between Yttria-Doped Ceria and Yttria-Stabilized Zirconia,” J. Solid State Chemistry, 129, 74-81 (1997).
[6] N. Q. Minh, “Ceramic Fuel Cells,” J. Am. Ceram. Soc., 76, 563-88(1993).

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