研究生: |
陳南宏 Nan-hung Chen |
---|---|
論文名稱: |
釤摻雜對二氧化鈰奈米顆粒之氧化還原行為及缺陷結構的影響 Effect of Sm Doping on the Redox Behavior and Defect Structure of Cerium Oxide Nanoparticles |
指導教授: |
陳詩芸
Shih-yun Chen |
口試委員: |
陳良益
Liang-yih Chen 宋振銘 Jenn-ming Song 郭永綱 Yung-kang Kuo |
學位類別: |
碩士 Master |
系所名稱: |
工程學院 - 材料科學與工程系 Department of Materials Science and Engineering |
論文出版年: | 2013 |
畢業學年度: | 101 |
語文別: | 中文 |
論文頁數: | 100 |
中文關鍵詞: | 二氧化鈰 、釤 、退火處理 、X光吸收光譜 、程式升溫還原 |
外文關鍵詞: | CeO2, Sm, annealing treatment, XAS, TPR |
相關次數: | 點閱:273 下載:1 |
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本研究利用沉澱法製備未摻雜、摻雜5at% Sm(釤)及摻雜11at% Sm(釤)之二氧化鈰奈米顆粒,並於300℃下不同氣氛(O2、Ar+H2)中進行退火處理,探討Sm之摻雜對二氧化鈰奈米顆粒之氧化還原行為的影響。此外,將經過氧化及還原退火處理之釤摻雜二氧化鈰(Sm-doped CeO2)進行程式升溫還原(TPR)分析,觀察不同缺陷含量之Sm-doped CeO2在不同溫度下與氫氣反應之情形,並可瞭解氧空缺之分佈情況。樣品之結構、粒徑及元素之價態則以X光繞射儀(XRD)、場發射穿透式電子顯微鏡(TEM),及X光吸收光譜(X-ray Absorption Spectroscopy,XAS)進行分析。
研究結果顯示:在氧化(O2)退火下,Sm之摻雜會不利於氧化(oxidation)反應之進行;在還原(Ar+H2)退火下,Sm之摻雜會提升還原(reduction)反應之能力。藉由TPR分析得知,5at% Sm經還原退火後之樣品,Sm3+傾向集中於結構內部。11at% Sm經氧化處理後,結構表層之Sm3+除了會促使還原反應之外,亦會使CeO2整體氧離子遷移率下降。
In this study, the undoped, 5at% Sm-doped and 11at% Sm-doped CeO2 nanoparticles were prepared by the co-precipitation methods. The samples were annealed in different atmospheres (O2, Ar+H2) at 300oC to discuss the effect of Sm doping on redox behavior of CeO2 nanoparticles. In addition, the Sm-doped CeO2 samples under different annealing treatment were analyzed via TPR(Temperature Programmed Reduction) to observe the relationship between temperature and H2 reaction. Furthermore, we can realize the distribution of oxygen vacancies by TPR analysis. The structure, particle size and elemental valence state of the sample were characterized by X-ray diffraction (XRD), field emission transmission electron microscopy (FETEM), and X-ray absorption spectroscopy (XAS).
The experimental results show that: under oxidative (O2) annealing treatment, the doping of Sm would be detrimental to the oxidation reaction. Under reductive (Ar+H2) annealing treatment, the doping of Sm would be beneficial to the reduction reaction. Through TPR analysis, the Sm3+ of 5at% Sm under reductive annealing treatment tend to aggregate in the bulk. However, the Sm3+ of 11at% Sm under oxidative annealing treatment tend to appear on the surface which is beneficial to the reductive reaction. Moreover, Sm3+ makes the oxygen mobility declined.
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