以氧化釓摻雜氧化鈰與氧化鉍混合行甲烷反應之研究

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研究生：	李家府 Jia-Fu Li
論文名稱：	以氧化釓摻雜氧化鈰與氧化鉍混合行甲烷反應之研究 Study of Methane Reaction with Gadolinia-doped Ceria Mixed Bismuth Oxide
指導教授：	黃大仁 Ta-Jen Huang
口試委員:
學位類別：	碩士 Master
系所名稱：	工學院 - 化學工程學系 Department of Chemical Engineering
論文出版年：	2007
畢業學年度：	95
語文別：	中文
論文頁數：	83
中文關鍵詞：	氧化鉍、氧化釓摻雜氧化鈰、甲烷、固熔
外文關鍵詞：	Bismuth oxide, Gadolinia-doped ceria, Methane, Solid solution
相關次數：	點閱：2 下載：0
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本研究主要是配合應用於直接甲烷固態氧化物燃料電池(Solid Oxide Fuel Cell﹐SOFC)的陽極甲烷反應，本研究選擇使用氧化釓添加氧化鈰( Gadolinia-doped Ceria﹐GDC )混合氧化鉍為材料，進行甲烷反應之研究。
藉由GDC提供的活性點、氧化鉍優異導氧離子性與反應選擇性，來增加二氧化碳的生成和減少積碳的產生，達到增加甲烷的轉化率。而本實驗根據EDX分析、XRD分析、程溫還原實驗和定溫甲烷反應的研究結果，以25wt%Bi2O3-GDC具有最好甲烷反應性。因為25wt%會有部分Bi2O3析出於GDC表面，但不會嚴重影響到GDC的內部結構，而降低內部晶格氧傳導的能力，且在預還原時可以減少GDC內部晶格氧的消耗與還原後增加甲烷反應的活性點。

目錄
第一章、緒論---------------------------------------------------------------------1
第二章、理論與文獻回顧------------------------------------------------------3
2-1導氧離子氧化物-------------------------------------------------3
        2-2氧空洞擔體------------------------------------------------------4
2-2-1固有缺陷擔體-------------------------------------------4
2-2-2非固有缺陷擔體----------------------------------------4
2-3 CeO2--------------------------------------------------------------6
2-4 氧化鉍----------------------------------------------------------7
2-4-1 δ-Bi2O3--------------------------------------------------9
2-5甲烷的相關反應式-------------------------------------------13
2-6積碳的生成與去除之方法----------------------------------17
2-7積碳-去積碳處理----------------------------------------------19
2-8觸媒擔體的選擇-----------------------------------------------22
第三章、實驗方法與步驟----------------------------------------------------23
3-1 實驗藥品-------------------------------------------------------23
3-2 製備方法-------------------------------------------------------23
3-2-1 氧化釓參雜氧化鈰-----------------------------------23
3-2-2 氧化鉍與氧化釓參雜氧化鈰混合-----------------24
3-3 實驗裝置與實驗方法----------------------------------------24
3-3-1 活性測試儀器----------------------------------------24
3-3-2 X-Ray 測量-------------------------------------------25
3-3-3 EDX測量----------------------------------------------25
3-3-4 BET表面積測量--------------------------------------25
3-3-5 程溫還原-----------------------------------------------25
3-3-6 程溫還原實驗-----------------------------------------26
3-3-6-1 H2-TPR實驗--------------------------------26
3-3-6-2 CO-TPR實驗-------------------------------26
3-3-6-2-1 無預還原-----------------------26
3-3-6-2-2 預還原--------------------------26
3-3-7甲烷程溫反應-----------------------------------------26
3-3-7-1 無預還原處理-----------------------------26
3-3-7-2 預還原處理--------------------------------27
3-3-8 定溫甲烷反應-----------------------------------------27
3-3-8-1無預還原處理------------------------------27
3-3-8-2預還原處理---------------------------------27
第四章、實驗結果與討論----------------------------------------------------32
4-1擔體的X光繞射分析-----------------------------------------32
4-2 EDAX分析------------------------------------------------------34
4-3 BET實驗---------------------------------------------------------35
4-4 H2-TPR與CO-TPR實驗--------------------------------------36
4-5預先還原處理再行CO-TPR實驗---------------------------42
4-6 甲烷程溫反應(CH4-TPRX) -----------------------------------44
4-6-1 經還原處理再行甲烷程溫實驗---------------------51
4-7 定溫甲烷反應---------------------------------------------------62
           4-7-1 不同溫度下的恆溫甲烷反應-----------------------73
           4-7-2 預還原處理後再行恆溫甲烷反應-----------75

第五章、結論--------------------------------------------------------------------79
第六章、未來展望-------------------------------------------------------------80第七章、參考文獻-------------------------------------------------------------81

                                

第七章、參考文獻
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