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  • 學位論文

添加劑對BaCeO3系質子導體導電率及穩定性之影響

The Effects of Dopant on Conductivity and Chemical Stability of BaCeO3-based Proton Conductors.

指導教授 : 洪逸明

摘要


本研究目的在探討陽離子摻雜對BaCeO3系質子導體導電率與相穩定性之影響。實驗採用固相反應法製備Ba1-xNxCe1-yMyO3-δ(N=Sr,M=Y, Sm)。以Y3+與Sm3+取代B位置,結果顯示:各成份導電率皆隨著溫度上升而增加,且以BaCe0.8Y0.2O3-δ導電率最高,於750 ℃、3 RH% (relative humidity)空氣下為0.026 S/cm;相較於BaCe1-ySmyO3-δ (0.019 S/cm)高出36.8 %。在750 ℃、3 RH % CO2環境下,BaCe0.8Y0.2O3-δ導電率為0.025 S/cm,與在3 RH%空氣下比較,其導電率下降了3.8 %。發現經過CO2環境處理後之BaCe1-yYyO3-δ,皆產生BaCO3與CeO2雜相,代表BaCe0.8Y0.2O3-δ已與CO2反應。在A位置摻雜對BaxCe1-ySmyO3-δ導電率影響方面,雖可製備 BaxCe1-ySmyO3-δ純相,但不論Ba2+離子增加或減少皆無法增加導電率。 在相穩定性方面,BaCe0.8Y0.2O3-δ優於BaCe0.8Sm0.2O3-δ,在80 ℃水氣環境處理4小時後僅有微量Ba(OH)2相產生。為了進一步增加Ba1-xNxCe1-yMyO3-δ穩定性,採用Sr2+取代Ba2+之方法。Ba0.9Sr0.1Ce0.8Y0.2O3-δ導電率在750 ℃、3 RH%空氣下,其導電度為0.023 S/cm,相較於BaCe0.8Y0.2O3-δ下降9.7 %。雖然摻雜Sr2+會使得導電率下降,但相穩定性明顯增加,在80 ℃水氣環境處理8小時後依然維持Ba0.9Sr0.1Ce0.8Y0.2O3-δ純相。 另外本研究亦探討粒徑大小對導電率之影響。利用Modified Pechini process可成功製備BaCe0.8Y0.2O3-δ奈米粉末,於900 ℃煆燒之粉體粒徑大小約為80 nm,導電率為0.025 S/cm,與固相反應法製備之微米BaCe0.8Y0.2O3-δ相當,並未明顯增加導電率。

並列摘要


The aim of this study was to investigate the influence of cation doped on conductivity and phase stability of BaCeO3-based proton conductors. Ba1-xNxCe1-yMyO3-δ (N=Sr, M=Y, Sm) were prepared by solid state reaction. For Y3+ and Sm3+ doped, BaCe0.8Y0.2O3-δ had the highest conductivity of 0.026 S/cm and higher 36.8 % than BaCe0.8Sm0.2O3-δ (0.019 S/cm) at 750 ℃ in 3 RH% (relative humidity) air atmosphere. The conductivity of BaCe0.8Y0.2O3-δ was 0.025 S/cm at 750 ℃ in 3 RH% CO2 environment which was lower 3.8 % than that at in 750 ℃ 3 RH% atmosphere. was produced BaCO3 and CeO2 impure phase after CO2 environment treatment in BaCe1-yYyO3-δ system, which meant BaCe1-yYyO3-δ reacted with CO2. Although pure BaxCe0.8Sm0.2O3-δ phase can be could prepare, they did not increase the conductivities in A site defect of BaCeO3-based proton conductors. The phase stability of BaCe0.8Y0.2O3-δ was better than BaCe0.8Sm0.2O3-δ. In this work, Sr2+ was doped in order to increase the phase stability of Ba1-xNxCe1-yMyO3-δ. Although the conductivity of Ba0.9Sr0.1Ce0.8Y0.2O3-δ was 0.023 S/cm at 750 ℃ in 3 RH% atmosphere which was lower 9.7 % than BaCe0.8Y0.2O3-δ, however, the phase stability of Ba0.9Sr0.1Ce0.8Y0.2O3-δ was much better than that of BaCe0.8Y0.2O3-δ. Nano BaCe0.8Y0.2O3-δ particle was prepared by modified Pehicni process with the particle size was about 80 nm. The conductivity was 0.025 S/cm which is similar to BaCe0.8Y0.2O3-δ prepared by solid state reaction.

並列關鍵字

SOFC electrolyte proton conductor BaCeO3

參考文獻


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