氧化鎳-鑭鍶鈷鐵奈米纖維陰極電極應用於質子傳導型固態氧化物電化學電池

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游易程(Yi-Cheng Yu) 查詢紙本館藏

畢業系所

材料科學與工程研究所

論文名稱

氧化鎳-鑭鍶鈷鐵奈米纖維陰極電極應用於質子傳導型固態氧化物電化學電池
(NiO-LSCF Nanofibrous Cathode Electrode for Proton-conducting Solid Oxide Electrochemical Cells)

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摘要(中)

質子傳輸型固態氧化物燃料電池(Proton-conducting solid oxide fuel cells, P-SOFCs)於工作溫度範圍(500-800 ℃)擁有優秀的質子傳導性、化學穩定性與電池密封性。但隨著工作溫度降低，會導致陰極電極的氧化還原能力(ORR)下降。由於NiO材料具有優秀的氧離子導率與表面氧交換能力，讓陰極電極側可以快速地解離氧氣和傳輸氧離子，以此有效提高電化學電池之性能，並且減少陰極電極之阻抗。
於本研究中，將使用不同X wt% NiO-LSCF (X=0, 10, 15, 20)奈米纖維作為P-SOFC的陰極電極。結果表示，NiO奈米顆粒在於LSCF纖維表面可以有效提升電池性能，因為NiO不僅擁有優良的離子導率，提供表面氧交換速率，其可以加速氧氣在形成氧離子過程中吸附、脫附與解離反應，以此來降低氧氣催化反應與氧離子傳輸到電解質界面處之極化阻抗。
15 wt% NiO-LSCF纖維電池於800°C 下進行性能測量，可得到最高功率密度約為477.6 mW/cm2，與純LSCF纖維電池相比高 18.5%，其原因為歐姆阻抗和極化阻抗分別降低了為26% 和71%。另一方面，在SOEC模式下進行15 wt% NiO-LSCF電解電池(Electrolyzer cell, EC)，先在陰極電極側電解水氣，而後在陽極電極側產生氫氣，法拉第效率(FE)與能量轉換效率(ECE)為69%與68%，其產氫的速率則為7.82 ml/min。
本研究結果顯示，15 wt% NiO-LSCF奈米纖維在P-SOFC中不僅擁有優秀的氧氣解離與氧離子傳輸之速率，於800 ℃下進行FC模式時，其電池之性能具有最高功率密度為477.6 mW/cm2。故15 wt% NiO-LSCF纖維電池成功應用於FC與EC模式，而15 wt% NiO-LSCF纖維陰極將提供P-SOFC裝置商業化發展之可能性。

摘要(英)

P-SOFCs have excellent proton conductivity, chemical stability, and better sealing in the operating temperature range (500-800 °C). However, with the operating temperature decreasing, the oxygen reduction reaction capability of the cathode electrode will be lower. Due to the superior oxygen-ionic conductivity and surface oxygen exchange capability of NiO nanoparticles, the cathode electrode will generate faster oxygen dissociation and offer the oxygen surface transport paths. NiO nanoparticles can effectively improve the electrochemical cell’s performance and reduce the cathode electrode’s impedance.
In this study, different content NiO such as X wt% NiO-LSCF (X=0, 10, 15, 20) nanofibers were used as the cathode electrode of P-SOFC. The results show that NiO nanoparticles on the surface of LSCF fibers can efficiently improve the performance of cell. NiO not only has excellent ionic conductivity and surface oxygen exchange rate but also accelerates the adsorption, desorption, and dissociation of oxygen. The NiO-LSCF nanofibrous cells will reduce the polarization resistance, which is about oxygen catalytic reaction and oxygen-ionic ‎transportation to the electrolyte interface.
At 800 °C, the performance test of the 15 wt% NiO-LSCF nanofibrous cell obtains a max. power density of 477.6 mW/cm2. It is higher 18.5% than the pure LSCF nanofibrous cell because ohmic impedance and polarization impedance are reduced by about 26% and 71%. In SOEC mode, the 15 wt% NiO-LSCF electrolyzer cell, which is H2O electrolysis at the cathode electrode and H2 generation at the anode electrode, has the Faraday′s efficiency and energy conversion efficiency of 69% and 68%. On the other hand, the hydrogen evolution rate of 15 wt% NiO-LSCF nanofiber cell is up to 7.82 ml/min.
This study shows that 15 wt% NiO-LSCF nanofibers not only have excellent oxygen dissociation and oxygen-ionic transportation rate in P-SOFC but also have a max. power density of 477.6 mW/cm2 at 800 °C. Therefore, 15 wt% NiO-LSCF cell has been successfully applied in FC and EC modes. The 15 wt% NiO-LSCF nanofibrous cathode will provide the possibility for commercial development of P-SOFC devices in the future.

關鍵字(中)

★ NiO-LSCF纖維
★ 複合纖維
★ 陰極電極
★ 表面氧交換
★ 固態氧化物燃料電池

關鍵字(英)

★ NiO-LSCF fibers
★ composite nanofibers
★ cathode electrode
★ surface oxygen exchange
★ P-SOFCs

論文目次

目錄
摘要 i
Abstract iii
目錄 vi
圖目錄 x
表目錄 xii
前言 1
第一章緒論 3
1.1. P-SOFC簡介 3
1.1.1. P-SOFC電池之工作原理 3
1.1.2. P-SOFC電池之結構 6
1.2. P-SOEC簡介 9
1.2.1. P-SOEC電池之工作原理 9
1.2.2. P-SOEC電池之結構 11
1.3. P-SOFC陰極材料與工作原理 12
1.3.1. 陰極材料介紹 12
1.3.2. 陰極表面修飾材料介紹 14
1.3.3. MIEC(MOEC)傳輸機制 15
1.3.4. 鈣鈦礦性質與結構 16
1.4. 纖維紡織技術 17
1.4.1. 纖維紡織原理 17
1.4.2. 纖維紡織參數 19
1.5. P-SOFC電解質之合成及燒結 21
1.5.1. P-SOFC電解質之粉末製作 22
1.5.2. 電解質燒結理論 22
1.6. P-SOFC電池製作 24
1.6.1. 電池乾壓成型 24
1.6.2. 電池刮刀成型 24
1.6.3. 電池旋轉塗佈 25
1.7. 電化學分析機制 26
1.7.1. 極化曲線工作原理 26
1.7.2. 阻抗頻譜工作原理 28
1.7.3. 擬合等效電路工作原理 29
第二章實驗方法 31
2.1 實驗藥品 31
2.2.　實驗方法與流程 32
2.2.1. 電池粉末合成 32
2.2.2. 刮刀塗佈製備陽極基板 33
2.2.3. 纖維陰極電極製作 34
2.2.4. 全電池製備 35
2.3.　材料分析儀器 37
2.3.1. X光粉末繞射儀(X-ray powder diffraction, XRPD) 37
2.3.2. 掃描式電子顯微鏡(Scanning electron microscopy, SEM) 38
2.3.3. 穿透式電子顯微鏡(Transmission Electron Microscopy, TEM) 38
2.4.　全電池I-V 性能之測量步驟 39
2.5.　阻抗頻譜之測量步驟 40
第三章實驗結果與討論 41
3.1.　全電池材料之相分析 41
3.1.1. 電解質材料之相分析 41
3.1.2. 電極材料之相分析 42
3.2.　電極材料之微結構分析 44
3.2.1. NiO-LSCF纖維陰極之表面分析 44
3.2.2. NiO-LSCF纖維陰極之截面分析 47
3.3.　全電池I-V 測量步驟與性能分析 49
3.4.　全電池之EIS測量步驟與阻抗分析 51
3.5.　全電池之穩定性分析 59
3.6.　全電池之法拉第效率與能量轉換效率分析 60
第四章結論 65
第五章參考文獻 67

圖目錄
圖1- 1：P-SOFCs可逆電化學裝置。 2
圖1- 2：O-SOFC/P-SOFC之操作原理示意圖。 4
圖1- 3：O-SOEC/P-SOEC之操作原理示意圖。 10
圖1- 4：P-SOFC陰極電極傳導示意圖。 13
圖1- 5：鈣鈦礦結構之示意圖。 17
圖1- 6：纖維紡織技術之示意圖。 18
圖1- 7：泰勒錐紡織過程之示意圖。 19
圖1- 8：前驅物表面電荷示意圖。 20
圖1- 9：粉末燒結之示意圖。 23
圖1- 10：乾壓成型之示意圖。 24
圖1- 11：刮刀成型之示意圖。 25
圖1- 12：旋轉塗佈之示意圖。 25
圖1- 13：典型燃料電池之極化I-V曲線圖。 28
圖1- 14：電化學阻抗複數平面示意圖。 29
圖2- 1：電解質粉末之合成流程圖。 33
圖2- 2：纖維紡絲技術之製程圖。 35
圖2- 3：半電池製作之流程圖。 36
圖2- 4：陰極電極製備之流程圖。 36
圖2- 5: P-SOFC測量步驟與平台示意圖。 40
圖3- 1：XRD圖於1250 ℃煆燒後BCZY622之電解質粉末。 41
圖3- 2：XRD圖於800 ℃ 煆燒後純LSCF nanofiber與15 wt% NiO-LSCF nanofiber。 43
圖3- 3：XRD圖 (a)電解質；(b)陽極電極。 44
圖3- 4：纖維陰極表面之SEM分析。 45
圖3- 5：15 wt% NiO-LSCF纖維之TEM分析。 46
圖3- 6：15 wt% NiO-LSCF奈米纖維EDS mapping之結果。 47
圖3- 7：纖維陰極截面之SEM影像分析。 48
圖3- 8：全電池之I-V曲線與功率密度測量結果。 50
圖3- 9：全電池電化學阻抗分析結果。 56
圖3- 10：NiO-LSCF奈米纖維電極之離子電子混合導體機制圖。 58
圖3- 11：15 wt% NiO-LSCF與LSCF之奈米纖維陰極於700 ℃進行24小時之長時間性能穩定性測試。 60
圖3- 12：15 wt% NiO-LSCF電池於800 ℃下，操作SOFC模式與SOEC模式之I-V曲線圖。 61
圖3- 13：15 wt% NiO-LSCF電池在800 ℃下，所測得之漏電流(圓形)與真實電解電流(三角形)。 62

表目錄
表1- 1：陰極材料之電子與離子導電率比較。 14
表1- 2：陰極材料之純氧離子導電率比較。 15
表1- 3：陰極電極之基本反應步驟。 15
表2- 1：實驗藥品對照表。 31
表2- 2：四種陰極電極組成參數。 37
表3- 1：四種陰極纖維電極組成參數。 48
表3- 2：四種陰極電極之電池阻抗。 57
表3- 3：15 wt% NiO-LSCF電池P-SOEC模式測得之數據表。 63
表3- 4：可逆循環反應能量轉換效率計算。 63

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指導教授

李勝偉(Sheng-Wei Lee)

審核日期

2022-8-23

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