臺灣博碩士論文加值系統

利用顯微拉曼光譜獲得在CO2環境下陶瓷粉末Ba(Zr0.8-xCexY0.2)O2.9(x=0.0-0.4)的振動模態。Ba(Zr0.8Y0.2)O2.9 和Ba(Zr0.6Ce0.2Y0.2)O2.9在低於1000 oC及CO2中展現很好的熱穩定性。然而，Ba(Zr0.5Ce0.3Y0.2)O2.9和Ba(Zr0.4Ce0.4Y0.2)O2.9只在550 oC以下表現出穩定性；在550 oC以上開始出現明顯的碳酸鋇和Zr0.8-xCexY0.2O2分解，可分別從拉曼譜峰1057和466 cm-1清楚地得到證實。本研究推測Ba(Zr0.8-xCexY0.2)O2.9陶瓷在x≤0.2的情況下，對於離子導體在含有二氧化碳的環境中之應用是很有前途的選擇。
以顯微拉曼散射來研究摻氟化鋰重量百分比7%的離子傳輸型陶瓷粉末Ba(Zr0.8-xCexY0.2)O2.9(x=0.1和0.2)在不同溫度的CO2環境中之穩定性。實驗發現摻氟化鋰會減低在CO2中的穩定性且在高溫CO2暴露後產生碳酸鋇以及可能是Ba3Ce2(CO3)5F2(或CeCO3F)和Y2O3-like的化合物。氟化鋰相關的化合物能在高於1200 oC的鍛燒(或燒結)後被消除，但Y2O3-like的化合物會被分解出來且在1400 oC大氣鍛燒後仍保留下來。

Atomic vibrations before and after exposure to CO2 were obtained for proton-conducting Ba(Zr0.8-xCexY0.2)O2.9 (x=0.0-0.4) ceramics by using micro-Raman scattering. Ba(Zr0.8Y0.2)O2.9 and Ba(Zr0.6Ce0.2Y0.2)O2.9 reveal a promising thermal stability in CO2 without apparent decomposition up to 1000 oC. However, Ba(Zr0.5Ce0.3Y0.2)O2.9 and Ba(Zr0.4Ce0.4Y0.2)O2.9 exhibit thermally stable below 550 oC and then proceed an obvious chemical decomposition of BaCO3 and Zr0.8-xCexY0.2O2 above 550 oC, which were clearly evidenced by the Raman vibrations of 1057 and 466 cm-1, respectively. The study suggests that the Ba(Zr0.8-xCexY0.2)O2.9 ceramics with x≤0.2 are promising candidates for proton-conducting applications in CO2-containing environment.
Micro-Raman scattering have been used to study thermal stability of lithium fluoride (LiF)-added (7% weight ratio) Ba(Zr0.8-xCexY0.2)O2.9 (BZCY : x=0.1 and 0.2) proton-conducting ceramic powders as a function of temperature in CO2. This work reveals that LiF-addition can reduce thermal stability of Ba(Zr0.8-xCexY0.2)O2.9 in 1 atm of flowing CO2 and causes decomposition to BaCO3, and possibly Ba3Ce2(CO3)5F2 (or CeCO3F), and Y2O3-like compound after exposure to CO2 from high temperature. LiF-related compounds can be removed after calcining (or sintering) in air above 1200 oC, but decomposition of Y2O3-like compound can be induced and remains after calcining in air at 1400 oC.

目錄
第一章 緒論 1
1.1研究動機與目的 1
1.2燃料電池的簡介與分類 1
1.3燃料電池的優點 2
1.4固態氧化物燃料電池的架構及工作原理 3
第二章 實驗原理-拉曼散射 7
2.1光散射 7
2.2古典電磁學理論基礎[10] 9
2.3微觀描述[9] 14
第三章 實驗儀器架構與樣品特性 17
3.1光路 17
3.2氬離子氣體雷射 19
3.3 J-Y U1000全像式雙光柵單色儀 23
3.4 CCD(電子耦合元件) 26
3.5 Ba(Zr0.8-xCexY0.2)O2.9陶瓷粉末 28
第四章 實驗結果與討論 31
4.1無氟化鋰BZCY顯微拉曼常溫光譜 31
4.2無氟化鋰BZCY顯微拉曼變溫光譜 36
4.3摻有氟化鋰BZCY顯微拉曼常溫光譜 49
第五章 結論 53
參考文獻 54

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