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    Please use this identifier to cite or link to this item: http://ir.lib.ncu.edu.tw/handle/987654321/4140

    Title: 稻殼灰分-氧化鋅複合擔體銅觸媒應用於甲醇部份氧化產氫之研究;Hydrogen Production by Partial Oxidation of Methanol over Cu/RHA-ZnO Catalysts
    Authors: 魏長青;Chung-Chung Wei
    Contributors: 化學工程與材料工程研究所
    Keywords: 銅觸媒;稻殼灰分-氧化鋅複合擔體;稻殼灰分;甲醇部份氧化反應;copper catalyst;RHA-ZnO binary support;hydrogen production;partial oxdation of methanol
    Date: 2009-06-22
    Issue Date: 2009-09-21 12:32:11 (UTC+8)
    Publisher: 國立中央大學圖書館
    Abstract: 本研究以初濕含浸法製備RHA-ZnO作為複合擔體,利用沉澱固著法使用銅金屬鹽類製備銅金屬觸媒,分別針對不同擔體比例條件、煅燒溫度、進料比例(O2/CH3OH)及反應溫度等變因進行討論。研究中利用熱重分析儀 (TGA)、X-ray繞射分析儀(XRD)、程式升溫還原(TPR)和穿透式電子顯微鏡(TEM)等儀器,分別對擔體或觸媒進行物性分析鑑定。以甲醇部份氧化反應(POM)探討各項操作變因對於甲醇轉化率、氫氣選擇率及一氧化碳選擇率之影響,目的在了解甲醇部份氧化反應產製氫氣及製備觸媒的最佳條件。 由XRD圖譜得知,Cu/RHA-ZnO (Si/Zn=9/1)的擔體比例為門檻,ZnO的含量越多,不只ZnO的繞射峰會越明顯,Cu的繞射峰也會變的明顯而有結晶狀態出現,而Si/Zn=9/1以下的擔體比例銅金屬則因粒徑太小無法在圖譜上可觀察到明顯波峰,而由Scherrer方程式所算出來的晶粒大小發現,ZnO的含量越多,銅的晶粒也隨之變大。而針對複合擔體觸媒Cu/RHA-ZnO (Si/Zn=9/1)做不同煅燒溫度的比較,XRD圖譜顯示煅燒溫度在573 K時並無法將硝酸銅鹽類完全分解,對照TGA圖譜和POM反應測試可知最佳煅燒溫度為673 K。 反應溫度低於448 K無法使反應進行,反應到達523 K時觸媒有最好的活性表現,最佳的反應物進料比為O2/CH3OH=0.3的比例。 In the research, we used the rice husk ash (RHA) and ZnO to prepare the binary support by incipient wetness impregnation method. After the binary support prepared, we deposited the copper metal on the binary support by deposite-precipitation method. N2O titration results indicated that the copper particle size increased with the increasing ZnO content in Cu/RHA-ZnO catalysts. The specific surface area of the reduced catalyst was increased with decreasing ZnO content. The catalysts showed higher activity after reduction. The active state of Cu/RHA-ZnO catalysts after reduction was Cu0 from XRD results. The dispersion of Cu/RHA-ZnO catalysts was decreased with increasing ZnO content. In XRD patterns and ICP-AES results, we could find that copper was precipitated on the support but it was too small to be detected on the support (Si/Zn, 9/1) which indicated that copper was highly dispersed on the support. Comparing with N2O titration results and TPR results, the catalyst reducibility depends on the copper particle size. We also found that Cu/RHA-ZnO (Si/Zn= 9/1) catalyst has more acid sites to improve the activity of partial oxidation of methanol. We calculated the copper particle size from TEM images and the average particle size of Cu/RHA-ZnO catalysts at 9/1(Si/Zn) atomic ratio was 3.5 nm. The appropriate calcination temperature is 673 K. When the ZnO content increased, the methanol conversion decreased slightly and the hydrogen selectivity decreased significantly. The feed ratio and appropriate reaction temperature were 0.3 and 523 K, respectively.
    Appears in Collections:[化學工程與材料工程研究所] 博碩士論文

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