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研究生: 林鴻穎
Lin-Hong-Ying
論文名稱: 催化材料與氧氣含量對乙醇蒸氣重組反應的影響
Effects of materials and oxygen contain on ethanol reforming reaction
指導教授: 王禎翰
學位類別: 碩士
Master
系所名稱: 化學系
Department of Chemistry
論文出版年: 2013
畢業學年度: 101
語文別: 中文
論文頁數: 98
中文關鍵詞: 乙醇蒸氣重組
英文關鍵詞: steam reforming
論文種類: 學術論文
相關次數: 點閱:108下載:6
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  • 本篇論文中,我們將有系統的研究十種金屬,(分別是 Ru 、 Rh 、 Ir 、 Co、Ni 、 Pd 、Pt 、 Cu 、 Au 和 Ag ),並將十種不同金屬分別附著在兩種不同金屬氧化支撐上,來進行氧化乙醇蒸氣重組反應,而這兩種氧化支撐物分別為,氧化鈰 (CeO2),和參雜了Dy的鈣鈦礦結構(Dy-doped BaZrO3)。在各種不同外在條件,如不同氧氣量的條件下(此篇氧氣量改變從0~40 sccm)、不同的溫度(此篇500℃~600℃)來進行實驗。這些使我們能夠了解整個乙醇蒸氣重組反應中,不同催化劑的性能以及它們對反應中所帶來的影響。在催化劑中金屬的部分,我們發現Rh、Ru、Ir這三種金屬,有助於C-C鍵斷裂,故產生最高的CO+CO2選擇率,並且有著最高的氫氣產率。 在催化劑中支撐物的部分,我們選擇了CeO2和鈣鈦礦結構(Dy-doped BaZrO3),這兩種支撐物可以分別有效的利用環境中氧氣與水,促使整個催化劑的效能提升。而其中鈣鈦礦結構(Dy-doped BaZrO3)效能提升特別明顯,是因為鈣鈦礦結構可以有效利用水,促使催化劑效能提升,所以可以看出水在乙醇蒸氣重組反應中具有重要的影響。在外在環境條件部分,我們發現增加溫度與氧氣含量,可以有效提升乙醇轉換效率、CO和CO2、氫氣產率。

    In this thesis, we systematically examine the examine the oxidative steam reforming of ethanol (OSRE) on 10 metals (Ru、Rh、Ir、Co、Ni、Pd、Pt、Cu、Au and Ag) supported on two oxide (CeO2、Dy-doped BaZrO3) at various operational conditions with different O2 flows (0 ~ 40 sccm) and temperatures (500℃~600℃) to elucidate the effects from catalysts and reagents on the catalytic performance. For metallic catalysts, we found that Rh, Ru, and Ir will improve C-C bond cleavage and produce mainly CO and CO2 with the highest hydrogen yield. For oxide supporters, both CeO2 and Dy-doped BaZrO3 that have high reactivity with oxygen and water, respectively, can further improve the catalytic performance. Especially, Dy-doped BaZrO3 shows the best enhancement, indicating that water plays an more important role in OSRE. For operational condition, we found that at high temperatures and oxygen contains can both improve ethanol conversion, CO and CO2 formation, and, eventually, raise the hydrogen yield.

    Key word : steam reforming

    第一章 : 緒論 1-1 介紹.....................................................................................................................13 1-2 乙醇重組反應的基本理論與現階段研究介紹.................................................14 第二章 : 實驗部分 2-1 實驗用藥品.........................................................................................................21 2-2 實驗用氣體.........................................................................................................23 2-3 實驗器材與儀器.................................................................................................24 2-4 催化劑的製備.....................................................................................................25 2-4-1 支撐物金屬前驅物用量.............................................................................25 2-4-2 金屬前驅物用量.........................................................................................25 2-4-3 製備催化劑.................................................................................................27 2-4-3-1 支撐物的製備......................................................................................27 2-4-3-2 含浸法(Impregnation)..........................................................................30 2-5 催化劑的特性鑑定.............................................................................................32 2-5-1 X光繞射分析(X-ray diffraction analysis,XRD)........................................32 2-5-2 能量散射光譜儀 (Energy dispersive X-ray spectroscopy EDS )..............33 2-6 活性測試及產物分析介紹.................................................................................34 6 2-7 管柱的活化與檢量線.........................................................................................37 2-7-1 管柱的活化(condition)...............................................................................37 2-7-2 檢量線的測定.............................................................................................38 2-8 乙醇重組活性測試.............................................................................................43 2-8-1 氫氣升溫還原程序.....................................................................................43 2-8-2 乙醇重組實驗.............................................................................................43 2-8-3 乙醇重組實驗之操作條件.........................................................................46 2-9 Gas Hour Space Velocity 、轉換效率與產率選擇率計算................................48 第三章 : 結果與討論 3-1 ex-situ 催化劑特性鑑定分析............................................................................50 3-1-1 XRD測試結果...............................................................................................50 3-1-2 Energy dispersive X-ray spectroscopy (EDS) 鑑定結果..............................51 3-2 溫度對十種金屬在不同支撐物上的影響.........................................................52 3-2-1 溫度對金屬附在不同支撐物上面(M/BZDy、M/CeO2)的影響...................69 3-2-2 氧氣含量對金屬附在不同支撐物上面(M/BZDy、M/CeO2)的影響..........77 3-2-3 十種金屬在不同支撐物上面(M/BZDy、M/CeO2)上的比較......................84 7 第四章 : 結論 4-1 結論.....................................................................................................................93 4-2 未來研究方向.....................................................................................................96 參考文獻......................................................................................................................97 關鍵字 : 乙醇轉氫重組

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    Key word : steam reforming

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