研究生: |
張混傑 HUN-CHIEH CHANG |
---|---|
論文名稱: |
氧化鈰薄層對鑭鍶鈷鐵氧/鑭鉬氧半電池之阻抗影響 The Influences of Ceria Thin Layer on Impedance of (LaSr)(CoFe)O3/LAMOX Half Cell |
指導教授: |
蔡大翔
Dah-Shyang Tsai |
口試委員: |
陳良益
Liang-Yih Chen 周振嘉 Chen-Chia Chou 鄭 淑 芬 Soofin Cheng |
學位類別: |
碩士 Master |
系所名稱: |
工程學院 - 化學工程系 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: | 105 |
中文關鍵詞: | 鑭鍶鈷鐵氧化物 、陰極 、固態氧化物電池 、氧還原反應 、鑭鏑鉬鎢氧化物 |
外文關鍵詞: | Lanthanum strontium cobalt ferrites, Cathode, Solid oxide fuel cell, Oxygen reduction reaction, Lanthanum dysprosium tungsten molybdate |
相關次數: | 點閱:262 下載:6 |
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本研究探討以鑭鍶鈷鐵氧化物(La1-ySry)(CoxFe1-x)O3 (y=0.1~0.4,x=0.1~0.9),作為匹配鑭鏑鉬鎢氧化物電解質(La1.8Dy0.2)(Mo1.6W0.4)O9 之陰極電化學表現,而因為鍶和鉬會反應生成SrMoO4,造成ORR阻抗的增加,所以使用SDC(Sm0.2Ce0.8O1.9)作為陰極和電解質之間的中間擋層,避免其直接接觸。然後以XRD、SEM分析材料結構,電化學交流阻抗分析圖譜儀及恆電位儀分析鑭鍶鈷鐵氧化物於塗有SDC層的鑭鏑鉬鎢氧化物電解質上之氧還原反應催化活性。
由XRD分析結果顯示,陰極材料為六方晶相之鈣鈦礦結構,無第二相存在,隨著鈷含量的增加,分峰的現象會變明顯。鑭鏑鉬鎢氧化物電解質(La1.8Dy0.2)(Mo1.6W0.4)O9的粉末與鑭鍶鈷鐵氧化物(La0.6Sr0.4)(Co0.8Fe0.2)O3的粉末混合後,恆溫800 ℃、6小時。經XRD分析,顯示有SrMoO4的生成。SEM的圖片上也可以看到SrMoO4的產生,尤其是在LSCF陰極和LDMW電解質的交界處。
SDC粉末膏網印於電解質兩面上,經燒結1000℃、2小時後,再將陰極粉末膏網印於塗有SDC中間層的電解質兩面上,經燒結800 ℃、2小時,顯微結構顯示陰極層為相當多孔之結構。以交流阻抗分析三極式對稱半電池之結果顯示,(La0.6Sr0.4)(Co0.8Fe0.2)O3-δ陰極組成在700 ℃下ASR(Area-specific resistance)達到最低為0.858 Ω•cm2。
利用對稱電池交流阻抗(impedance)所量測到的RLF以及CorrView商用軟體進行回歸計算求得交換電流密度,兩種方法求得的值相近,在(La0.6Sr0.4) (Co0.8Fe0.2)O3-δ之陰極組成,其交換電流密度700 ℃時達18.3 mA/cm2。
In this work, we study the cathode performance of (La1-ySry)(CoxFe1-x)O3 (y=0.1~0.4,x=0.1~0.9) LSCF coupled with the electrolyte (La1.8Dy0.2)(Mo1.6W0.4)O9 LDMW. A (Sm0.2Ce0.8)O1.9 SDC layer is applied between cathode and electrolyte to impede the interdiffusion between Sr and Mo, which produces SrMoO4 and drastically increase the oxygen reduction reaction (ORR) resistance. The structure and morphology are investigated using X-ray diffraction XRD and scanning electron microscopy SEM. The electrochemical performance is focused on the ORR loss measured on the symmetric electrode of half cell using impedance spectroscopy and Tafel plot recorded by a potentiostat.
The XRD results indicate that the LSCF cathode possesses perovskite structure of rhombohedral cell, no secondary phase detected. With increasing Co content, several diffraction peaks begin to split. The phase of SrMoO4 has been detected in the mixture of LSCF and LDMW after heating at 800℃ for 6 h. A dense product layer has also been observed between the LSCF cathode and LDMW electrolyte in the SEM micrograph.
The half cell of symmetric electrode has been prepared by coating the LDMW electrolyte on both sides with SDC paste and sintered at 1000℃ for 2h, then coating LSCF on both sides and sintered at 800℃ for 2h. The impedance spectroscopy analysis indicates that (La0.6Sr0.4)(Co0.8Fe0.2)O3 exhibits the minimum ORR resistance, 0.858 Ω•cm2 at 700℃.
The measured ORR resistance by impedance spectroscopy is consistent with the ion exchange current density measured by CorrView software. The ion exchange current density is 18.3 mA/cm2 at 700℃.
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