中文質子傳輸型固態氧化物燃料電池陽極之研究

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龐又齊(Yu-Chi Pang) 查詢紙本館藏

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能源工程研究所

論文名稱

中文質子傳輸型固態氧化物燃料電池陽極之研究
(Synthesis and Investigation of Anode for Medium Temperature Proton Exchange Solid Oxide Fuel Cell Research)

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摘要(中)

本研究主要探討利用固相反應法(Solid State Reaction, SSR)製作合金陽極應用在質子傳輸型固態氧化物燃料電池(Proton Conducting Solid Oxide Fuel Cell, P-SOFC)。合金陽極量測則分為成份比例、晶相鑑定、微觀結構、機械性質及電性分析；藉由調整鎳鈷合金(Nickel Cobolt Alloy, NiCo alloy)的煆燒溫度、煆燒時間及改變NiCo合金比例，目標是以少許鈷元素(Cobalt, Co)與鎳元素(Nickel, Ni)置換之陽極達到比傳統以Ni金屬為主之陽極具有較佳之電性、抗碳沉積能力及氧化還原循環穩定性。
研究結果顯示，藉由調整NiCo合金粉末煆燒溫度及煆燒時間會改變NiCo合金晶粒大小、導電度及熱膨脹係數。當Ni0.9Co0.1合金之煆燒溫度為1000 ºC及煆燒時間為3小時，操作溫度為600 ºC時，其導電度為2623 S/cm。選取最佳煆燒溫度、煆燒時間及NiCo成份比例，當Ni : Co莫爾比為9:1時，陽極具有相當優異之導電度及熱膨脹係數，其導電度比傳統以金屬Ni為主之陽極高，當Ni : Co莫爾比為7:3時，其熱膨脹係數為13.6×10-6 K-1、有最佳的抗碳沉積能力及經過氧化還原循環後有最佳機械強度。

摘要(英)

In this research, solid-state reaction (SSR) synthesis process is chosen to develop an alloy catalyst as an anode in proton conducting solid oxide fuel cell (P-SOFC). Initially, anode alloy is characterized to identify the ratio of components, phase identification, microstructure, mechanical properties and electrical conductivity. The aim of this research is to synthesize a higher electrical conducting anode catalyst for P-SOFC, when compared to the traditional NiO anode. Incorporation of cobalt in nickel oxide can enhance the electrical properties of anode in P-SOFC. Several variations in the ratio of alloy (Ni : Co) and calcining parameters such as temperature and time would enhance the electrical conductivity, carbon deposition resistance and the redox cycle stability of the catalyst. This is better than the traditional NiO catalyst. The results show that, variation of calcined temperature and calcined time can change the particle size, electrical conductivity and coefficient of thermal expansion (CTE). Initially, we investigated the best appropriate calcination temperature and duration, and then the ratio of Ni : Co is varied. The best carbon deposition resistance, stability in redox cycle and CTE of 13.6×10-6 K-1 is observed for the Ni : Co molar ratio of 7 : 3. The NiCo anode has relatively good electrical conductivity than that of Ni anode (2354 S/cm). This work can help to replace the traditional NiO anode in P-SOFC.

關鍵字(中)

★ 中溫
★ 質子傳導
★ 固態氧化物燃料電池
★ 熱膨脹係數
★ 維克氏硬度
★ 碳沉積
★ 氧化還原循環

關鍵字(英)

★ Intermediate Temperature
★ Proton Conduction
★ Solid Oxide Fuel Cell
★ Coefficient of Thermal Expansion
★ Vickers Hardness
★ Carbon Deposition
★ Redox Cycle

論文目次

中文摘要 i
Abstract ii
致謝 iii
目錄 iv
圖目錄 vii
表目錄 x
一、緒論 1
1-1 前言 1
1-2 固態氧化物燃料電池(SOFC) 2
1-2-1 P-SOFC及O-SOFC 3
1-2-1 P-SOFC工作原理 4
1-3 P-SOFC材料具備之特性 5
1-3-1 P-SOFC電解質 6
1-3-2 P-SOFC陽極材料 9
二、文獻回顧 12
2-1 鋇鈰氧系(BaCeO3-based)陽極材料之穩定性問題 12
2-2 改變煆燒溫度對於合金顆粒的影響 15
2-3 改變合金比例對於陽極材料性質的影響 17
三、實驗方法 21
3-1 實驗製程儀器設備 21
3-1-1 行星式單罐球磨機 21
3-1-2 桌上型油壓機 21
3-1-3 高溫箱型爐 21
3-2 實驗樣品製備流程 21
3-2-1 陽極製備流程 21
3-3 材料分析儀器 23
3-3-1 X光繞射儀(X-Ray Diffraction, XRD) 23
3-3-2 掃描式電子顯微鏡(Scanning Electron Microscope, SEM) 24
3-3-3 熱機械分析儀(Thermomechanical Analysis, TMA) 25
3-3-4 維克氏硬度試驗機(Vickers Hardness Testing Machine) 26
3-3-5 波長分散式X光螢光分析儀(Wavelength Dispersive X-ray Fluorescence, WD-XRF) 26
3-3-6 同步熱差分析儀(Simultaneous Thermal Analysis, STA) 27
3-3-7 導電度阻抗儀(Impedance Analyzer) 28
3-3-8 拉曼光譜儀(Raman Spectrometer) 29
3-3-9 元素分析儀(Elemental Analyzer, EA) 30
四、結果與討論 31
4-1 不同煆燒溫度對陽極材料之影響 31
4-1-1 不同煆燒溫度陽極之樣品命名 31
4-1-2 不同煆燒溫度對陽極材料比例、形貌及導電度之影響 31
4-2 不同煆燒時間對陽極材料之影響 35
4-2-1 不同煆燒時間之樣品命名 35
4-2-2 不同煆燒時間對陽極材料比例、形貌及導電度之影響 36
4-2-3 不同煆燒溫度及煆燒時間對陽極晶粒大小、孔隙率及導電度之影響整理 39
4-3 不同比例NiCo合金對陽極材料之影響 40
4-3-1 不同比例NiCo合金之樣品命名 40
4-3-2 不同比例NiCo合金對陽極材料比例、形貌、導電度、硬度及熱膨脹係數之影響 40
4-3-3 不同比例NiCo合金陽極塊材之碳沉積實驗 46
4-3-4 不同比例NiCo合金陽極塊材之氧化還原循環實驗 50
4-3-5 不同合金比例對陽極晶粒大小、孔隙率、導電度、熱膨脹係數、抗碳沉積能力與氧化還原循環耐受性之影響整理 58
五、結論 60
六、未來工作 61
七、參考文獻 62

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指導教授

曾重仁(Chung-Jen Tseng)

審核日期

2019-8-20

推文