質子傳輸型固態氧化物燃料電池之水電解電化學性能量測與探討

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戴國瑜(Kuo-Yu Tai) 查詢紙本館藏

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材料科學與工程研究所

論文名稱

質子傳輸型固態氧化物燃料電池之水電解電化學性能量測與探討
(Electrochemical Performance on Water Electrolysis of Protonic Ceramic Electrochemical Cells)

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摘要(中)

可逆固態氧化物電池(Reversible Solid Oxide Fuel Cells, R-SOFCs)為一種兼具發電與儲能功能的可逆燃料電池。SOEC在高溫下電解水氣並以氫能進行電力儲存，待需要電力時再將氫能進行SOFC轉換成電力使用。該方法可以避免再生能源之間歇性發電，導致電力可能發生輸出斷層，即可有效提升可再生能源的產量。另外，此裝置可視為一個既穩定又乾淨的系統，並同時降低溫室氣體排放量，因為副產物僅有水氣，可當作新世代的潔淨能源。
在本實驗研究中，將探討LSCF以及GCCCO作為固態氧化物燃料電池之空氣電極材料，以及通過使用旋轉塗佈以及脈衝雷射技術製備空氣電極功能層的方法，探討其單電池於R-SOFC下的性能。LSCF作為空氣電極具有良好的電子與氧離子傳導能力，且在中溫操作下具有足夠高的雙向輸出性能；而GCCCO具有良好的電子、氧離子及質子之傳輸能力，可以在中溫下進一步提升R-SOFC性能。另外，將透過改變空氣電極功能層的製備方法，進一步降低歐姆和極化阻抗，使得單電池之能量密度以及電流轉換效率進一步地提升。因此本實驗研究將建立一套可靠的燃料電池(FC)與電解電池(EC)的測量方法以及數據分析，並在不同測量溫度下探討其電化學性能。
本實驗研究顯示，透過PLD製備空氣電極功能層的GCCCO單電池，其FC模式在800 ℃下的最高功率密度為962.4 mW/cm2，與旋轉塗佈製備的LSCF單電池相比高了128 %，其原因為歐姆阻抗以及極化阻抗分別降低了54 %和85 %。而PLD製備空氣電極功能層的GCCCO單電池在EC模式下，其產氫量為3.31E-06 g/s以及其法拉第效率為41.5 %，相對旋轉塗佈製備的LSCF單電池而言僅有25.7 %。

摘要(英)

Operation of Reversible Solid Oxide Fuel Cells (R-SOFCs) have both power generation mode (SOFC) and energy storage mode (SOEC). SOEC electrolyzes water vapor at high temperature and stores electricity as hydrogen energy. When the times as electricity is needed, hydrogen is then converted into electricity by SOFC mode. In this way, the characteristics of intermittent power when generating electricity by renewable energy can be avoided, which may cause electricity output faults if more electricity was required at busy times. In addition, this device can be regarded as a stable and clean system as water vapor is the only by-product, which may also reduce greenhouse gas emissions.
In this study, the performance of LSCF and GCCCO as air electrode in R-SOFC, alongside with different methods of preparing interlayer, spin coating and PLD, were explored. As an air electrode, both LSCF and GCCCO has good electron and oxygen ion conductivities, and also shows good performance in R-SOFC at medium temperature. However, GCCCO can also conduct protons, which may further increase the performance of R-SOFC. Furthermore, the ohmic and polarization resistance will be further reduced by changing the preparation method of the interlayer. Hence, the maximum power density and Faradic efficiency of a single cell can be further improved. Moreover, a reliable measurement method will be established in both FC and EC mode in this study, as well as its electrochemical data analysis on different temperatures will be discussed.
This experimental study shows that the maximum power density of the GCCCO single cell prepared by PLD interlayer at 800°C in FC mode is 962.4 mW/cm2, which is 128 % higher than the LSCF single cell prepared by spin coating interlayer. Because the ohmic and polarization impedance are reduced by about 54 % and 85 % respectively. In EC mode, the GCCCO single cell prepared by PLD interlayer has a hydrogen production rate of 3.31E-06 g/s and its Faradaic efficiency of 41.5 %. In comparison, the Faradaic efficiency of LSCF single cell prepared by spin coating has only 25.7%.

關鍵字(中)

★ 可逆固態氧化物電池
★ 燃料電池
★ 電解電池
★ 旋轉塗佈技術
★ 脈衝雷射沉積技術
★ 空氣電極功能層
★ LSCF
★ GCCCO

關鍵字(英)

★ Reversible Solid Oxide Fuel Cells (R-SOFC)
★ fuel cells
★ electrolysis cells
★ spin coating
★ pulsed laser deposition
★ interlayer
★ LSCF
★ GCCCO

論文目次

摘要 VI
Abstract VIII
致謝 X
目錄 XI
圖目錄 XIV
表目錄 XVII
第一章、前言 1
第二章、實驗原理及文獻回顧 3
2.1 燃料電池簡介 3
2.2 質子傳輸型固態氧化物燃料電池 5
2.2.1質子傳輸型固態氧化物燃料電池之原理 5
2.2.2質子傳輸型固態氧化物燃料電池之結構 7
2.3質子傳輸型固態氧化物電解電池 9
2.3.1質子傳輸型固態氧化物電解電池之原理 9
2.3.2質子傳輸型固態氧化物電解電池之結構 10
2.3.3水電解原理 10
2.3.4電解電流原理 13
2.3.5漏電流原理 14
2.3.6產氫量分析 15
2.4空氣電極材料與傳輸機制 17
2.4.1空氣電極種類介紹 17
2.4.2 MIEC傳輸機制 19
2.4.3鈣鈦礦(Perovskite)結構及性質 20
2.4.4三重導體原理及傳輸機制 22
2.5空氣電極功能層 24
2.5.1空氣電極功能層之原理 24
2.5.2以脈衝雷射技術製備空氣電極功能層 25
2.6電化學分析原理 27
2.6.1極化曲線(I-V curve)之原理 27
2.6.2電化學交流阻抗頻譜之原理 29
2.6.3等效電路之簡介 31
2.7電池製備技術 33
2.7.1乾壓成型技術(Dry pressing technique) 33
2.7.2刮刀成型技術(Tape casting technique) 33
2.7.3旋轉塗佈技術(Spin coating technique) 34
2.7.4脈衝雷射沉積技術(Pulsed Laser Deposition technique) 35
2.8 研究動機及目的 36
第三章、實驗方法 37
3.1實驗藥品 37
3.2實驗方法及流程 38
3.2.1粉末合成 38
3.2.2刮刀成型技術製備陽極基板 39
3.2.3旋轉塗佈技術製備半電池 40
3.2.4旋轉塗佈技術製備LSCF空氣電極功能層全電池 41
3.2.5脈衝雷射沉積技術製備GCCCO空氣電極功能層全電池 42
3.3材料性質分析 45
3.3.1 X光粉末繞射儀 45
3.3.2掃描式電子顯微鏡(Scanning electron microscopy, SEM) 45
3.3.3氣相層析儀(Gas Chromatography, GC) 46
3.4單電池I-V性能量測 48
3.5電化學交流阻抗分析 49
3.6單電池之電解水產氫分析 49
3.6.1 GC檢量線製作 49
3.6.2量測漏電流 51
3.6.3量測總電流 51
3.6.4量測產氫量與法拉第效率 51
第四章、結果與討論 53
4.1材料相分析 53
4.1.1電解質粉末之相分析 53
4.1.2單電池之相分析 54
4.2單電池之I-V性能量測與分析 55
4.3單電池之EIS量測與分析 57
4.4單電池之電解水產氫量測與分析 61
第五章、結論 68
第六章、參考文獻 69

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指導教授

李勝偉

審核日期

2024-1-30

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