脈衝雷射沉積技術製作薄膜質子傳輸型固態氧化物燃料電池

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林怡婕(Y-Jie Lin) 查詢紙本館藏

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材料科學與工程研究所

論文名稱

脈衝雷射沉積技術製作薄膜質子傳輸型固態氧化物燃料電池
(Fabrication of thin-film proton–conducting solid oxide fuel cells by using pulsed laser deposition)

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摘要(中)

現今許多研究在致力於將固態氧化燃料電池的操作溫度降低，並希望以減少電解質的厚度來獲得較高的電池電性。為有效降低電解質厚度，本實驗利用雷射脈衝沉積法，製備以BaCe0.6Zr0.2Y0.2O3-δ為基礎之電解質，此氧化物在中溫(600-800℃)範圍內具有穩定之質子傳導性，可降低操作溫度，製備出的電解質的厚度可下降到小於5 μm，縮短質子傳遞路徑，且具有柱狀紋理的微結構，可降低晶界電阻。為製備良好的電解質層，在不同的基板加熱溫度下，進行雷射鍍膜，並觀察其顯微結構以及利用XRD進行成相分析，藉此找到適合做為固態氧化燃料電池的電解質之鍍膜參數，並以此參數進行電池製備。在基板上製備電解質層前，為填補兩層間的孔洞，並降低因材料上的不匹配會產生薄膜附著性差的問題，先以雷射脈衝沉積法鍍上陽極功能層，再進行電解質製備。陰極的製作是使用雷射脈衝沉積法，製作具有孔洞的La0.6Sr0.4Co0.2Fe0.8O3-δ。完整的電池具有陽極(基板)、陽極功能層、電解質、陰極四層結構，對電池進行電池能量密度的量測，並觀察電池的顯微結構。為降低電解質與陽極間的孔洞與分離情形，加入退火等步驟，以改善電池電化學表現及能量密度。但昇降溫的步驟會造成電解質的龜裂，因此去除退火步驟，避免裂縫阻擋質子傳輸，進而提升電池效能。

摘要(英)

Solid oxide fuel cells (SOFCs) have drawn significant attention owing to their high efficiency. Reducing the SOFC operating temperature can be achieved by preparing thin film electrolytes. In this work, SOFCs with thin BaCe0.6Zr0.2Y0.2O3-δ (BCZY) electrolytes were fabricated by pulsed laser deposition (PLD). The thickness of BCZY could be reduced to about 3 μm.The NiO- BaCe0.6Zr0.2Y0.2O3-δ (NiO-BCZY) which played the role of anode functional layers were deposited on NiO-BCZY anode supports by PLD due to the surface pores of supports might cause defects during electrolyte deposition. After reduction of NiO to Ni at 800℃, the anode functional layers became porous while preserve fine adhesion with electrolyte. This study has also investigated the microstructure morphologies of La0.6Sr0.4Co0.2Fe0.8 (LSCF) cathode films via the PLD process. LSCF films deposited at 600℃ under 100 mtorr of oxygen pressure have dense structure when those films deposited at room temperature under the same background pressure have porous structure. A single cell had four layers : anode substrate、anode functional layer、electrolyte and cathode. The single cell with four layer and without post-annealing after deposition of each layer generated maximum power densities of 38.3 mWcm?2 at 800 °C and open circuit voltage of 0.9 V.

關鍵字(中)

★ 雷射脈衝沉積法
★ 固態氧化物燃料電池
★ 電解質
★ 陽極功能層

關鍵字(英)

★ pulsed laser deposition
★ SOFC
★ proton-conducting
★ electrolyte
★ anode functional layer

論文目次

摘要 i
Abstract ii
致謝 iii
目錄 iv
圖目錄 vii
表目錄 ix
第一章緒論 1
1.1 燃料電池簡介 1
1.2 固態氧化物燃料電池 (SOFC) 2
1.2.1 SOFC之原理[6-9] 3
1.2.2 SOFC之優缺點 4
1.2.3 SOFC之陽極探討 5
1.2.4 SOFC之陰極探討 5
1.2.5 SOFC之電解質探討 6
1.3 脈衝雷射沉積技術 7
1.3.1 脈衝雷射沉積技術原理 7
1.3.2 PLD雷射源種類 7
1.3.3 PLD的優缺點 8
1.3.4 薄膜沉積原理 9
1.4 文獻回顧 10
1.5 研究動機 12
第二章實驗流程 13
2.1 實驗流程 13
2.2 靶材製備 13
2.3 陽極基板製備 14
2.4 脈衝雷射沉積系統 14
2.4.1 真空腔體 14
2.4.2 鍍膜氣體環境 15
2.4.3 雷射源 16
2.4.4 雷射光路 17
2.4.5 靶材載台 18
2.4.6 基板載台 19
2.4.7 Fluence 計算 20
2.4.8 鍍率計算與校正 21
2.5 分析儀器 23
2.5.1 X光繞射 (X-Ray Diffraction) 23
2.5.2 掃描式電子顯微鏡 (Scanning Electron Microscopy) 23
2.5.3 電解質能量密度測量 23
2.5.4 電化學阻抗頻譜法(EIS) 24
第三章結果與討論 25
3.1 材料分析 25
3.1.1 陽極基板 25
3.1.2 以PLD製作NiO-BCZY 27
3.1.3 以PLD製作BCZY 29
3.1.4 以PLD製作LSCF 32
3.2 電池量測 34
3.2.1 電性量測 36
3.2.2 EIS測量 38
3.3 結論 39
3.4 未來展望 39
第四章參考資料 40

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指導教授

李勝偉

審核日期

2018-8-23

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