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研究生： 陳俞璁
Yu-Tsung Chen
論文名稱： NO在Perovskite oxide上的分解反應之研究
指導教授： 楊思明
Sze-Ming Yang
口試委員:
學位類別： 碩士
Master
系所名稱： 工學院 - 化學工程與材料工程學系
Department of Chemical & Materials Engineering
畢業學年度： 89
語文別： 中文
論文頁數： 84
中文關鍵詞： EXAFS 、XANES 、O2-TPD 、Perovskite 、NO分解反應
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    • 本論文主要使用sol-gel方法合成Perovskite觸媒，進行NO分解催化反應，利用氧氣程溫脫附實驗來分析Perovskite的氧氣脫附性質，及以X光吸收光譜術來分析La1-xSrxMO3(M=Co﹑Mn﹑Fe﹑Ni)與LaCoyMn1-yO3中，Co﹑Mn﹑Fe﹑Ni的周圍環境。
    Perovskite型混合氧化物﹐具有高熱穩定性﹐對CO﹑碳氫化合物具有良好氧化力﹐對NO的分解也有相當的活性﹐加上價格較低廉﹐遂有取代原本貴重金屬支撐在氧化鋁上的研究價值。本篇論文發現La1-xSrxMO3（M = Co﹑Fe﹑Mn﹑Cr）中Sr取代量增加，可以提升NO分解反應活性，尤其是低溫區的反應活性。經過Mn部份取代Co而成的LaCo0.9Mn0.1O3與LaCoO3相比有較高的低溫反應活性。
    利用氧氣程溫脫附分析及X光吸收光譜分析分別可以解釋Perovskite觸媒氧空缺及A﹑B位置元素部份取代的Perovskite觸媒對NO分解反應活性的變化趨勢。

    In this study, Perovskite oxides synthesized by sol-gel method are used as the catalyst for NO decomposition reaction. Oxygen desorption propreties of Preovskite are studied by O2-TPD experiments. The local environments around Co, Mn, Fe and Ni ions are examined by means of X-ray absorption spectroscopy of LaMO3(M=Co, Mn, Fe, Ni) and LaCoyMn1-yO3.
    Results indicate partially substitution of La by Sr in Perovskite oxides and by a small amount of Mn in LaCoO3 can improve the activity of NO decomposition.
    The results of O2-TPD show that the amounts of desorbed oxygen between 300 to 600℃(α´peak) increases with increasing amount of Sr substitution for La in Perovskite oxides. X-ray absorption spectroscopy results show decrease of coordination numbers when Sr substitutes La. Oxygen vancancies are generated by partial substitution of La by Sr. The increase of activity for NO decomposition can be attributed to the increase of oxygen vancancies upon substitution.

    目 錄 中文摘要……………………………………………………………Ⅳ 英文摘要………………………………………………………..…Ⅴ 圖目錄……………………………………………………………..Ⅵ 表目錄……………………………………………………………..Ⅸ 第一章 緒論…………………………………………………………1 1.1 前言…………………………………………………………….1 1.2 Perovskite型觸媒簡介………….…………………………..3 1.3 X光吸收光譜術簡介………………………………………….16 第二章 實驗方法………………………………………………….22 2.1 藥品與氣體…………………………………………...…….22 2.2 實驗儀器………………………………………………………23 2.3 Perovskite oxide觸媒之製備…………………….………….24 2.4 Perovskite oxide觸媒之結構鑑定…………….…………….24 2.5 比表面積(BET)分析…………………………………………..24 2.6 氧氣程溫脫附(O2-TPD)………………………………………25 2.7 一氧化氮分解反應催化活性測試……………………………26 2.8 X光吸收光譜術測量方法………………………………..….27 2.9 X光吸收光譜術數據分析步驟……...………………………30 第三章 結果與討論……………………………………………………32 3.1 晶相結構分析…………………………………………………32 3.2 比表面積(BET)測量…………………………………………..33 3.3 一氧化氮分解反應催化活性測試……………………………38 3.4 氧氣程溫脫附(O2-TPD)……………………...……………….46 3.4-1 Sr取代La的影響………………..……………….….46 3.4-2 B位置元素(Ni﹑Co﹑Mn﹑Fe﹑Cr)的影響…….……49 3.4-3 Co﹑Mn互相取代的影響 ………………………….…51 3.5 X光吸收光譜結果分析……………..…………….………56 3.5-1 X光近吸收邊緣（XANES）分析……………………..56 3.5-1.1 Co K-吸收邊緣之XANES….………………...56 3.5-1.2 Mn K-吸收邊緣之XANES…………………...61 3.5-1.3 Fe與Ni K-吸收邊緣之XANES……………64 3.5-2 延伸X光吸收細微結構（EXAFS）分析………..…….66 3.5-2.1 Co K-吸收邊緣之EXAFS……………………….66 3.5-2.2 Mn K-吸收邊緣之EXAFS……….………………71 3.5-2.3 Fe K-吸收邊緣之EXAFS………….…………….76 3.5-2.4 Ni K-吸收邊緣之EXAFS………………………..79 第四章 結論………………………………………………………..…..82 第五章 參考文獻…………………………………………..…………84

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