碳酸鹽沉澱製備Ba0.5Sr0.5Co0.8Fe0.2O3 及其在滲透銀前後之陰極特性比較

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許皓妮(Hao-ni Hsu) 查詢紙本館藏

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論文名稱

碳酸鹽沉澱製備Ba0.5Sr0.5Co0.8Fe0.2O3 及其在滲透銀前後之陰極特性比較
(Precipitation of carbonate to prepare Ba0.5Sr0.5Co0.8Fe0.2O3 and its cathodic character before and after treatment with Ag-diffusion)

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摘要(中)

本論文以含特定濃度之鋇、鍶、鈷與鐵等硝酸鹽溶液，加入碳酸銨溶液，在控制pH下，共沉獲得Ba0.5Sr0.5Co0.8Fe0.2O3 (BSCF氧化物)之碳酸鹽前驅物，經不同溫度煆燒所得粉末材料，製成固態氧化物燃料電池陰極，研究其結晶性質、表面形貌、電化學性質等，探討作為燃料電池陰極觸媒之可行性。結果顯示：含0.1M硝酸鋇、0.1M硝酸鍶、0.16M硝酸鈷與0.04M硝酸鐵溶液在加入飽和碳酸銨溶液，滴定至滴定終點為pH 8.0，過濾後得沉澱物，經1000℃煆燒2小時後獲得粉末，製成電池陰極。由場發射電子顯微鏡(FE-SEM)觀察陰極材料表面，顯示為多孔結構；X光繞射光譜儀(XRD)鑑定粉末晶體結構，顯示為純屬鈣鈦礦結構的Ba0.5Sr0.5Co0.8Fe0.2O3，未出現其他相。此種氧化物，經加入硝酸銀加溫，形成銀顆粒附著在BSCF氧化物顆粒上，所製成之固態氧化物燃料電池之陰極，其孔隙率由38.89 %降至33.74 %，因而影響到其陰極行為。

摘要(英)

Carbonate precursor of Ba0.5Sr0.5Co0.8Fe0.2O3 (BSCF oxide) was prepared by chemical precipitation from a nitrate solution containing specific concentrations of barium, strongnium, cobalt and iron to react with a saturated solution of ammonium carbonate at various pH values. After filtration, the precipitate was calcined at different temperatures to form Ba0.5Sr0.5Co0.8Fe0.2O3 (BSCF oxide) powder that in turn was fabricated as the cathode catalyst. The surface morphology, crystalline structure and electrochemical property of the cathode catalyst were investigated prior to and post treatment with silver nitrate at elevated temperatures to estimate its cathodic catalyst used in the solid oxide fuel cells (SOFC). Resulting from chemical precipitation of a nitrate solution containing 0.1 M barium, 0.1 M strongnium, 0.16 M cobalt and 0.04 M iron reacted with a saturated solution of ammonium carbonate at pH equal to 8.0, the precipitate was filtered out, dried and calcined at 1000℃ for 2 h to attain the oxide powder. Through examination of FE-SEM, the calcined oxide revealed a porous morphology. Analysis of x-ray diffraction (XRD) displayed that the crystal of the oxide belonged to a perovskite of Ba0.5Sr0.5Co0.8Fe0.2O3 without presence of any detectable impurity. The oxide powder was fabricated into cathode catalyst which was treated with silver nitrate at elevated temperatures to study the effect of this treatment. Silver particles were coated on the BSCF oxide. It was found that the cathode catalyst decreased the porosity from 38.89% to 33.74 % after the treatment. It will influence its cathodic reactivity.

關鍵字(中)

★ 固態氧化物燃料電池
★ 陰極
★ 催化劑
★ 化學共沉澱法
★ 滲透法
★ 電化學

關鍵字(英)

★ SOFC
★ Cathode
★ Catalyst
★ Chemical co-precipitation method
★ Permeation method
★ Electrochemistry

論文目次

中文摘要 i
Abstract ii
致謝 iv
目錄 v
表目錄 ix
圖目錄 x
第一章簡介 1
1.1 研究背景 1
1.2 研究動機 3
1.3研究目的與目標 4
第二章原理與文獻回顧 5
2.1固態氧化物燃料電池簡介 5
2.2固態氧化物燃料電池原理 7
2.3陰極材料之性質 9
2.3.1鈣鈦礦結構 10
2.3.2陰極材料 10
2.4固態氧化物電池材料常用合成法 12
2.5電池測試原理 16
2.6文獻回顧 19
2.6.1 SOFC陰極材料文獻回顧 19
2.6.2電化學交流阻抗文獻回顧 22
第三章實驗方法 26
3.1實驗藥品與材料 26
3.2樣品準備與製程 26
3.2.1 BSCF陰極粉末製備 26
3.2.2黏結劑與陰極膏製備 27
3.2.3半電池製備 28
3.2.4含銀之改質陰極製備 29
3.3儀器分析設備 29
3.3.1 X光繞射儀（X-Ray Diffractormeter, XRD） 29
3.3.2場發射電子顯微鏡（FE-SEM） 30
3.3.3感應耦合電漿質譜分析儀（ICP-MS） 31
3.3.4熱重分析儀（TGA） 31
3.3.5孔隙率量測 32
3.3.6電導率量測 33
第四章研究結果 34
4.1碳酸鹽共沉法製備BSCF陰極粉末 34
4.1.1煆燒溫度對BSCF粉末結構與形貌之影響 34
4.1.2 pH值對BSCF粉末結構與形貌之影響 37
4.1.3粉末ICP-MS分析 37
4.1.4粉末熱重分析 38
4.2陰極性質分析 38
4.2.1陰極層孔隙率量測 38
4.2.2陰極表面與斷面SEM分析 39
4.2.3陰極材料之電導率量測分析 40
第五章討論 42
5.1 BSCF中成份之溶解度積與pH值關係 42
5.1.1沉澱劑選擇對結晶結構之影響 42
5.1.2表面微結構分析 43
5.2 BSCF摻銀前後之特性探討 44
第六章結論 45
參考文獻 47

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指導教授

林景崎(Jing-chie Lin)

審核日期

2013-8-28

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