臺灣博碩士論文加值系統

本論文研製之中溫型固態氧化物燃料電池(IT-SOFC)，進一步發展為雙向固態氧化物燃料電池(URSOFC)，具有進行SOFC與SOEC雙向模式的能力。
本研究所採用電池為TLC法製備的陽極支撐型鈕扣電池，陽極材料為多孔氧化鎳(NiO-YSZ)，並使用鑭鍶鈷鐵(LSCF)作為陰極材料。鑭鍶鈷鐵是相對於鑭鍶錳(LSM)有較高電子電導率與良好離子電導率的混合離子電子導體。但是在高溫下會與電解質YSZ產生不導電相如：La2Zr2O7、SrZrO3。
為了避免此現象發生，本研究致力於研究GDC interlayer的燒結製程，將GDC interlayer燒結在1200-1300度之間，並在中溫型固態氧化物電池的工作溫度下(700 ℃-850 ℃)做性能測試。在SOFC與SOEC模式下完成性能測試後，藉由SEM分析電池在測試前後所產生的微結構變化。
最後我們發現，燒結在1300度的GDC interlayer電池，在850度下具有最大的功率密度288.578 (mW/cm2)。在850 ℃下有28.54 %的性能提升。GDC interlayer除了在放電模式下可以提升傳統電池性能外，在電解模式一樣可以有更大的增幅。本實驗設計皆是在氫氣極相對濕度80 %下進行測試。其中性能具有最大增幅的是GDC interlayer燒結在1250度的電池，在850 ℃下2.0 V時具有最大電解電流648.464 (mA/cm2)。相較於傳統電池，電解性能有386%的性能提升。

A procedure is mainly study the intermediate temperature solid oxide fuel cell (IT-SOFC), and further develop it into Utilized Regenerative solid oxide fuel cell (URSOFC), which has the capability of SOFC and SOEC bidirectional mode.
In this study, an anode supported button cell was prepared by TLC method. The anode material was porous nickel oxide (NiO-YSZ) and lanthanum strontium cobalt ferrite (LSCF) was used as the cathode material. The lanthanum strontium cobalt ferrite is a mixed ionic electronic conductor with respect to the lanthanum strontium manganese (LSM) with higher electrical conductivity and good ionic conductivity. But at high temperatures with the electrolyte YSZ produce non-conductive phase such as: La2Zr2O7、SrZrO3.
In order to avoid this phenomenon, we devoted to study of GDC interlayer sintering process, and GDC interlayer sintered between 1200-1300 degrees. And test at 700-850 degrees to know the chemical performance. We used SEM to know the cell microstructure changed after SOFC mode and SOEC mode.
Finally, we found that the GDC interlayer sintered at 1300 degrees had a maximum power density of 288.578 (mW/cm2) at operation temperature 850 °C. And one of the biggest increases in performance is the GDC interlayer sintered at 1250 degrees with a maximum current density 648.464 (mA / cm2) at 2.0 V at 850 °C.
Compared to traditional SOFC, electrolysis performance will get 386% performance improvement.

目錄
GDC INTERLAYER對於SOEC與SOFC性能之研究 I
論文口試委員審定書 II
元智大學博碩士論文授權書 III
誌謝 VIII
目錄 IX
表目錄 XII
圖目錄 XIII
1.1雙向固態氧化物燃料電池 (UNITIZED REGENERATIVE SOLID OXIDE FUEL CELL，URSOFC)簡介 1
1.2研究動機 3
1.3文獻回顧 4
二、 固態氧化物燃料電池結構 9
2.1固態氧化物燃料電池結構 9
2.1.1單電池夾具設計 10
2.2氫氣極支撐型電池 11
2.2.1氫氣極 11
2.2.2電解質 13
2.2.3氧氣極 14
2.3密封材料 15
三、 實驗設備與方法 19
3.1實驗設備與方法 19
3.2實驗目的與設計 20
3.3 固態氧化物燃料電池燒結 21
3.4 電池測試升溫與活化測試程序 23
3.5 GDC INTERLAYER與氧氣極燒結製程 24
3.6 SOFC模式下添加GDC INTERLAYER與否之性能差異 25
3.7 SOEC模式下添加GDC INTERLAYER與否之性能差異 27
3.8 SEM照攝 28
四、 結果與討論 30
4.1 GDC INTERLAYER燒結製程 30
4.2 SOFC模式下添加GDC INTERLAYER與否之性能差異 30
4.3 SOEC模式下添加GDC INTERLAYER與否之性能差異 33
4.4 SEM照攝 36
五、 結論 37
I. GDC INTERLAYER燒結 37
II. SOFC模式下添加GDC INTERLAYER性能提升 37
III. SOEC模式下添加GDC INTERLAYER性能提升 38
IV. SEM照攝 38
六、 未來規劃 39
I. 製程改善 39
II. 夾具改善 39
參考文獻 40

1. V.A.C. Haanappel and A. Mai, J. Mertens, Electrode activation of anode-supported SOFCs with LSM- or LSCF-type cathodes, Solid State Ionics, 177, pp. 2033–2037 (2006).
2. Wi-Heon Kim, Hwa-Seob Song, Jooho Moon and Hae-Won Lee, Intermediate temperature solid oxide fuel cell using (La,Sr)(Co,Fe)O3-based cathodes, Solid State Ionics, 177, pp. 3211–3216 (2006).
3. Gianfranco DiGiuseppe and Li Sun, Electrochemical performance of a solid oxide fuel cell with an LSCF cathode under different oxygen concentrations, International Journal of Hydrogen Energy 36, pp.5076－5087 (2011).
4. Jeong Woo Yun, Jonghee Han, Sung Pil Yoon, Sanggyun Park, Hee Su Kim and Suk Woo Namb, Ce0.8Gd0.2O2 modification on La0.6Sr0.4Co0.2Fe0.8O3 cathode for improving a cell performance in intermediate temperature solid oxide fuel cells, Journal of Industrial and Engineering Chemistry 17, pp. 439–444 (2011).
5. Sun Jae Kim and Gyeong Man Choi, Stability of LSCF electrode with GDC interlayer in YSZ-based solid oxide electrolysis cell, Solid State Ionics, 262, pp. 303–306 (2014).
6. Seung-Young Park, Jee Hyun Ahn, Chang-Woo Jeong, Chan Woong Na, Rak-Hyun Song and Jong-Heun Lee, Ni-YSZ-supported tubular solid oxide fuel cells with GDC interlayer between YSZ electrolyte and LSCF cathode, International Journal of Hydrogen Energy 39,pp. 12894－12903 (2014).
7. Hyun-Jong Choi, Young-Hm Na, Doo-Won Seo, Sang-Kuk Woo and Sun-Dong Kim, Densification of gadolinia-doped ceria diffusion barriers for SOECs and IT-SOFCs by a sol–gel process, Ceramics International, 42, pp. 545–550 (2016).
8. Muhammad Zubair Khan, Muhammad Taqi Mehrana, Rak-Hyun Song, Jong-Won Lee, Seung-Bok Lee, Tak-Hyoung Lim and Seok-Joo Park, Effect of GDC interlayer thickness on durability of solid oxide fuel cell cathode, Ceramics International, 42, pp.6978-6984 (2016).
9. Sun Jae Kima, Sun Woong Kim, Young Min Park, Kun Joong Kim and Gyeong Man Choi, Effect of Gd-doped ceria interlayer on the stability of solid oxide electrolysis cell, Solid State Ionics, 295, pp. 25–31 (2016).
10. Peter Styring, Elsje Alessandra Quadrelli and Katy Armstrong, Carbon Dioxide Utilisation Closing the Carbon Cycle, ELSEVIER (2015).
11. Frano Barbir, Angelo Basile and T. Nejat Vezirog˘ lu,Compendium of Hydrogen Energy Volume 3:Hydrogen Energy Conversion, ELSEVIER (2016).