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姓名	賴星魁(Shin-Quei Lai)  查詢紙本館藏	畢業系所	化學工程與材料工程學系
論文名稱	CuO/CeO2/MnOx/Al2O3觸媒於富氫環境下對CO選擇性氧化反應研究 (Selective oxidation of CO in excess hydrogen over CuO/CeO2/MnOx/Al2O3 catalysts)
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摘要(中)	本研究以共沉澱法製得Ce1-xMnxO2擔體，再以含浸法製備10% CuO/Ce1-xMnxO2觸媒，藉以了解Mnn+引入CeO2對PROX反應的影響。另採工業觸媒常用的共沉澱法製備CuO/CeO2/MnOx/Al2O3觸媒，探討各成分比例對PROX反應的影響與作用。PROX反應於進料氣體比CO/O/H2/He = 1/1/50/48及質流比F/W = 10,000 mlh-1gcat-1下進行，並採用BET、TPR、Raman、XPS、Auger與脈衝式CO吸附等分析方法探討觸媒之物理特性與表面性質。 10% CuO/Ce1-xMnxO2觸媒中，Mnn+引入可進入CeO2晶格中形成Ce-Mn-O固溶物，增加擔體redox特性，引入量可達到x = 0.3而不使觸媒活性降低。共沉澱法可製得高CuO負載量且分散良好的CuO/CeO2/ MnOx/Al2O3觸媒，最適的煅燒溫度為650°C 。CuO/CeO2觸媒之CuO負載量可高達30%，而不影響T100 (90~95°C)。MnOx引入CuO/CeO2中，亦可形成固溶物，MnOx的引入不僅可協助CeO2的redox特性，MnOx本身亦扮演與CuO交互作用的協同角色，引入量可高達30%，而T100略升為95~100°C。Al2O3的引入雖可增強觸媒物理性質，但引入量不宜超過10%。CuO/CeO2/MnOx/Al2O3觸媒活性取決於CuO與CeO2是否良好接觸，各成分的引入量過多會發生聚集分離，降低CuO與CeO2接觸機會，而不利於反應，最理想的組成比例為30/40/20/10。CuO/CeO2/MnOx/Al2O3 (30/40/20/10)觸媒具有媲美CuO/CeO2與CuO/Ce1-xMnxO2觸媒的活性與選擇性，且可處理高容量的反應氣體，進料中引入CO2 與H2O雖會使觸媒活性與選擇率下降，但觸媒仍具有相當良好的穩定性，是具實用性的理想PROX反應之觸媒。
摘要(英)	In order to realize the effect of PROX reaction when Mnn+ was incorporated into CeO2, Ce1-xMnxO2 mixed oxides were prepared as supports of 10% CuO/Ce1-xMnxO2 catalysts which prepared by impregnation method. Then CuO/CeO2/MnOx/Al2O3 catalysts were prepared by co-precipitation method for use in the PROX reaction. The effects of CuO/CeO2, MnOx/CeO2, and MnOx/Al2O3 on the selective oxidation of CO were examined and the roles of CeO2, MnOx and Al2O3 were discussed. The feed H2/CO/O2/He (50/1/1/48) were diverted to the reactor at the flow rate of 30 ml/min (F/W = 10,000 mlh-1gcat-1). The physical and surface properties of catalysts were determined by BET, XRD, TPR, XPS and pulsing adsorption of CO. For Ce1-xMnxO2, Mnn+ incorporated into the CeO2 lattice to form Ce-Mn-O solid solution and enhanced redox properties of supports for CuO/Ce1-xMnxO2 catalysts. The incorporated amount of Mnn+ could be achieved x = 0.3 without weakened activity. It could obtain high CuO loading and fine dispersion CuO/CeO2/MnOx/Al2O3 catalysts by co-precipitation method when the optimum calcinations temperature was 650°C. CuO loading amount could be as high as 30%, and the temperature (T100) for complete conversion was about 90~95oC. Introducing MnOx into CuO/CeO2 could also form Ce-Mn-O solid solution. MnOx would not only increase the mobility of lattice oxygen but also played a synergistic role interacting with CuO. Therefore, The selective oxidation of CO was not weakened as part of CeO2 replaced by MnOx less than 30%, while slightly increased T100 for 95~100°C. Incorporating Al2O3 weakened the activity. Nevertheless, an appropriate amount of Al2O3 (10%) was needed for the physical properties of the catalysts. CuO/CeO2/MnOx/Al2O3 (30/40/20/10) catalyst exhibited a good activity and a good selectivity that was comparable with CuO/CeO2 and 10% CuO/Ce1-xMnxO2, and can handle high-capacity gas. The activity and selectivity of catalysts decrease in the presence of CO2 and H2O, but it still showed good stability. It is a practical and ideal catalyst for PROX reaction.
關鍵字(中)	★ 一氧化碳選擇性氧化 ★ 氧化錳 ★ 銅鈰觸媒	關鍵字(英)	★ MnOx ★ CeO2.PROX ★ CuO
論文目次	中文摘要 i 英文摘要 ii 誌 謝 iv 目 錄 vi 圖目錄 ix 表目錄 xii 第一章 緒論 1 第二章 文獻回顧 3 2-1 PROX反應之觸媒 4 2-1-1 Pt觸媒 4 2-1-2 Ru、Rh、Pd、Ir觸媒 7 2-1-3 Au觸媒 9 2-1-4 CoOx觸媒與CuO觸媒 12 2-2 CeO2與CuO/CeO2觸媒特性 14 2-2-1 CeO2 14 2-2-2 CuO/CeO2觸媒於PROX反應之表現 17 2-2-3 CuO/CeO2觸媒作用機制 19 2-3 CuO/ Ce1-xMexO2觸媒 22 2-3-1 Ce1-xZrxO2共氧化物與CuO/Ce1-xZrxO2觸媒 22 2-3-2 Ce1-xSnxO2共氧化物與CuO/Ce1-xSnxO2觸媒 24 2-3-3 其它促進劑 25 2-4 MnOx、CuO-MnOx、CeO2-MnOx氧化物 27 2-4-1 MnOx 27 2-4-2 CuO-MnOx spinel結構氧化物 28 2-4-3 CeO2-MnOx共氧化物 29 第三章 實驗方法與設備 34 3-1觸媒製備 34 3-1-1 CuO/Ce1-xMnxO2 觸媒之製備 34 3-1-2 CuO/CeO2/MnOx/Al2O3觸媒之製備 35 3-2 觸媒性質鑑定 36 3-2-1 比表面積測定(BET) 36 3-2-2 X-射線繞射分析(XRD) 37 3-2-3 X-射線光電子光譜(XPS) 37 3-2-4 氫-程溫還原(H2-TPR) 38 3-2-5 脈衝式CO吸附 39 3-3富氫下CO選擇性氧化反應研究 40 3-4 CO2與H2O影響實驗 41 3-5 轉化率與選擇率之計算 41 3-6 實驗藥品與氣體 44 第四章 結果與討論 45 4-1 CuO/Ce1-xMnxO2觸媒 45 4-1-1 Ce1-xMnxO2擔體XRD結構分析 45 4-1-2 Ce1-xMnxO2擔體結構之拉曼(Raman)分析 46 4-1-3 Ce1-xMnxO2擔體氫程溫還原(TPR) 49 4-1-4 觸媒活性測試與討論 49 4-2 CuO/CeO2/MnOx/Al2O3觸媒 54 4-2-1 煅燒溫度的影響 54 4-2-2 CuO/CeO2比例的影響 58 4-2-2 CeO2/MnOx比例對CuO/CeO2/MnOx觸媒的影響 70 4-2-3 MnOx/Al2O3比例對CuO/CeO2/MnOx/Al2O3觸媒的影響 81 4-3改變F/W對CuO/CeO2/MnOx/Al2O3(30/40/20/10)觸媒的影響 92 4-4 CO2與H2O對PROX反應之影響 95 4-5 200小時反應穩定性測試 95 第五章 結論 99 總 結 101 參考文獻 102
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指導教授	陳吟足(Yin-Zu Chen)	審核日期	2009-7-23
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