鑭鏑鉬氧電解質之單室固態氧化物燃料電池的功率提升

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研究生：	姚志杰 Chih-chieh Yao
論文名稱：	鑭鏑鉬氧電解質之單室固態氧化物燃料電池的功率提升 Power improvement of single chamber SOFC with (La1.8Dy0.2)Mo2O9 electrolyte
指導教授：	蔡大翔 Dah-Shyang Tsai
口試委員:	周振嘉 Chen-Chia Chou 鄭淑芬 Soo-fin, 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：	2011
畢業學年度：	99
語文別：	中文
論文頁數：	115
中文關鍵詞：	鑭鉬氧電解質、單氣室、固態氧化物燃料電池、梯度式陰極、梯度式陽極、甲烷燃料
外文關鍵詞：	Lanthanum molybdate electrolyte, Single chamber, SOFC, Gradient cathode, Gradient anode, methane fuel
相關次數：	點閱：248 下載：0
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先前我們實驗室已證實鑭鏑鉬氧化物((La1.8Dy0.2)Mo2O9)作為固態氧化物燃料電池之電解質，此燃料電池目前可以可運用在中溫範圍單氣室條件下工作。本研究藉由梯度式陰、陽極調整其與電解質匹配性提升電池電功率密度表現。
在提升功率表現的工作上，主要分為兩階段:第一階段以找出最佳化的電解質厚度、陽極孔洞率及陰極的結構與厚度，並以LDM為電解質， GDC(Ce0.9Gd0.1O1.95) + LDM +Ni為陽極，SSC(Sm0.5Sr0.5CoO3) + GDC為陰極。當電解質、陽極與陰極的組成固定時，以63 m電解質、25m梯度式SSC+GDC陰極與500 mm GDC+LDM+Ni(含10 wt.%石墨)陽極所製備之電池，於700 C下，進料氣體體積流量為350 sccm且比例為甲烷與氧氣1.5:1時，擁有電功率密度329.9 mW/cm2。
第二階段在相同的量測條件下，著重於改善陽極部分，藉由梯度式陽極、添加陽極功能層(AFL)與添加Pd 觸媒。所有在此階段量測的電池其電解質厚度皆為632 m、梯度式陰極厚度皆為252 m，而雙層梯度式陽極將電池電功率密度提升至377.8 mW/cm2，而將電功率密度提升主要歸因於在外層陽極中添加20 wt.% 石墨增加孔洞率，以致降低濃度極化阻抗提升電功率密度表現。之後，為了增加陽極與電解質介面間的三相點數，因而添加一層粒徑較小之功能層，其所製備之電池電功率密度更進一步提升至388.1 mW/cm2。添加Pd觸媒部分，發現僅於外層陽極添加Pd觸媒比內層陽極添加效果較佳，且僅於外層陽極添加3 wt.%Pd時所製備之電池電功率密度達437.3 mW/cm2。

The previous studies of this research group have demonstrated La1.8Dy0.2Mo2O9 (LDM) is a feasible electrolyte for solid oxide fuel cell (SOFC), operating under single chamber conditions in intermediate temperature range. In this work, we further uplift the power performance of this SOFC through upgrading its matching anode and cathode.
The efforts are divided in two phases in improving the power performance. Phase I, we optimize the electrolyte thickness, the anode porosity, and the cathode microstructure and thickness, while LDM is the electrolyte, GDC(Ce0.9Gd0.1O1.95) + LDM + Ni is the anode, SSC(Sm0.5Sr0.5CoO3) + GDC is the cathode. When the compositions for electrolyte, anode, and cathode are fixed, the optimal single chamber power is read at 700 C, with 63 m thick LDM, 25 m thick gradient cathode of SSC + GDC, and 0.5 mm thick porous anode of GDC + LDM + Ni including 10 wt%graphite as pore former. The peak power value of the optimal cell measures 329.9 mW/cm2, in a 350 sccm flow of methane and air mixture with the CH4 : O2 ratio 1.5:1.
In phase II, we focus on the anode improvement, including application of gradient anode, addition of anode functional layer (AFL), and addition of palladium catalyst, while fixing the single chamber operation conditions. All the test cells in phase II were prepared with an electrolyte of 632 m in thickness and a gradient cathode of 252 m in thickness. A two-layer anode uplifts the peak power value to 377.8 mW/cm2, and we attribute the improvement to the more porous (20wt% graphite) outer layer which reduces the concentration polarization. The cell performance is further enhanced to the power level of 388.1 mW/cm2, after adding a functional layer between anode and electrolyte to increase the triple-phase boundary. Addition of palladium catalyst in anode is found effective in the outer layer, not the inner layer. And 3 wt% Pd catalyst in outer anode lifts the peak power value to 437.3 mW/cm2.

摘要	I
ABSTRACT	III
目錄	V
圖目錄	X
表目錄	XV
第一章 序論	1
1-1 前言	1
1-2研究動機	3
第二章 文獻回顧與理論基礎	4
2-1燃料電池簡介	4
2-2固態氧化物燃料電池基本原理	8
2-2-1 雙氣室固態氧化物燃料電池(DC-SOFC)	9
2-1-2 單氣室固態氧化物燃料電池(SC-SOFC)	11
2-3 固態氧化燃料電池陽極	13
2-3-1 氧化鋯鎳基陽極	14
2-3-2 氧化鈰鎳基陽極	15
2-3-3 鈣鈦礦結構陽極材料	16
2-3-4 La2Mo2O9系電解質的配合陽極	17
2-4 固態氧化物燃料電池的電解質	19
2-4-1 氧化鋯(Zr2O)基電解質	21
2-4-2 氧化鈰(CeO2)基電解質	23
2-4-3 鎵酸鑭 (LaGaO3)基電解質	24
2-4-4 氧化鉍(Bi2O3)基電解質	25
2-4-5 鑭鉬氧化物(La2Mo2O9)電解質	27
2-4-5-1 鑭鉬氧化物( La2Mo2O9 )其氧離子導機制	28
2-4-5-2 鑭鉬氧化物(La2Mo2O9)優缺點	29
2-5 固態氧化燃料電池陰極	32
2-6 電極改質	36
2-6-1 孔洞生成劑	37
2-6-2 功能層與梯度結構電極	38
2-6-3 陽極摻雜貴金屬	40
2-7 固態氧化物燃料電池之極化現象	41
2-7-1 歐姆極化	42
2-7-2 濃度極化	43
2-7-3 活化極化	44
2-8 粉體製備	45
第三章 實驗方法與步驟	48
3-1 實驗方法	48
3-2 實驗藥品	50
3-3 儀器設備	52
3-4 電池元件的製備	54
3-4-1 製備 (La1.8Dy0.2)Mo2O9 電解質粉末	54
3-4-2 製備NiO、 (Ce0.9Gd0.1)O1.95與 (Sm0.5Sr0.5)CoO3粉末	56
3-4-3 製備陽極基材 ( NiO – (Ce0.9Gd0.1)O1.95 – (La1.8Dy0.2)Mo2O9 - 孔洞生成劑 )	60
3-4-4 調製電池元件用膠	62
3-4-5 製備陰極電極	63
3-4-6 製備電流收集器	64
3-5 燃料電池之特性鑑定與分析	64
3-5-1 SEM 表面影像分析	64
3-5-2交流阻抗分析	65
3-5-2 熱膨脹係數分析	65
3-6 燃料電池之測試	66
3-6-1 測試系統簡介	66
3-6-2 電池電流-電壓測試流程	67
第四章 結果與討論	68
4-1 XRD結構鑑定與分析	69
4-1-1 陰極晶體結構鑑定	69
4-1-2 陰極氫氣還原XRD分析	71
4-2 陽極添加孔洞生成劑	72
4-2-1 SEM分析	73
4-2-2電功率密度測試	75
4-3 不同厚度之電解質與陰極	77
4-3-1 不同厚度之電解質	77
4-3-1-1 SEM分析	77
4-3-1-2電功率密度測試	78
4-3-1-3 交流阻抗分析	80
4-3-2 不同厚度之陰極	82
4-3-2-1 SEM分析	82
4-3-2-2電功率密度測試	83
4-3-2-3交流阻抗分析	84
4-3-2-4 陰極熱膨脹係數匹配	86
4-4 梯度材料及功能層之陽極	89
4-4-1 梯度材料與孔洞率之陽極	91
4-4-1-1 SEM分析	91
4-4-1-2電功率密度測試	93
4-4-1-3交流阻抗分析	94
4-4-2 功能層之陽極	95
4-4-2-1 SEM分析	95
4-4-2-2電功率密度測試	96
4-4-2-3交流阻抗分析	96
4-5 陽極摻雜貴金屬	98
4-5-1 梯度式陽極摻雜 1 wt% Pd	98
4-5-1-1 電功率密度測試	98
4-5-1-2 交流阻抗分析	100
4-5-2 梯度式陽極摻雜不同含量 Pd	101
4-5-2-1 電功率密度測試	101
4-5-2-2 交流阻抗分析	103
第五章 結論	106
參考文獻	109
附錄A	115

                                

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