添加氧化鋯促進劑的稻殼灰分擔體銅觸媒應用於甲醇部份氧化產氫之研究; Effects of ZrO2-promoter on catalytic performance of Cu RHA catalysts for production of hydrogen by partial oxidation of methanol

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Title:	添加氧化鋯促進劑的稻殼灰分擔體銅觸媒應用於甲醇部份氧化產氫之研究;Effects of ZrO2-promoter on catalytic performance of Cu RHA catalysts for production of hydrogen by partial oxidation of methanol
Authors:	林惠聰;Hui-tsung Lin
Contributors:	化學工程與材料工程研究所
Keywords:	銅觸媒;氧化鋯;稻殼灰分;甲醇部份氧化產氫;Cu catalyst;Zirconia;partial oxidation of methanol
Date:	2010-07-06
Issue Date:	2010-12-08 13:35:48 (UTC+8)
Publisher:	國立中央大學
Abstract:	本研究以沉澱固著法製備含ZrO2促進劑的銅金屬觸媒，分別探討ZrO2含量、煅燒溫度、進料比例(O2/CH3OH)及反應溫度等變因對觸媒活性的影響，目標為評估所製備觸媒的效能並找出最佳操作條件。研究中利用感應耦合電漿原子放射光譜儀(ICP-AES)、熱重分析儀(TGA)、X-ray繞射分析儀(XRD)、N2O解離吸附(N2O titration)、程式升溫還原(TPR)和穿透式電子顯微鏡(TEM)等儀器，分別對各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。由XRD圖譜得知，含有ZrO2的觸媒，其Cu的繞射峰會有減弱趨勢，而且在高溫煅燒下，抗燒結能力也會大幅提升。N2O及TEM結果顯示，ZrO2的存在可提高Cu在擔體上的分散度，使Cu顆粒的粒徑維持在5 nm以下。TGA的結果提供了煅燒溫度的參考範圍，對照POM活性測試可知最佳煅燒溫度為673 K，而最佳的反應物進料比為O2/CH3OH=0.3，反應溫度為523 K時觸媒有最好的活性表現。 Using rice husk ash (RHA) as support, we prepared the Cu catalysts by deposition-precipitation method. ZrO2 was added as promoter to Cu/Zr/RHA catalysts and these nano-catalysts were tested for hydrogen production by partial oxidation of methanol to identify the activity. A detail study for physical property of Cu/Zr/RHA catalysts was analyzed by ICP-AES, TGA, XRD, N2O titration, TEM, and TPR. XRD results indicated that the copper diffraction peak of Cu/Zr/RHA was weaker than Cu/RHA, and the Cu diffraction peak would not increase with higher calcination temperature. It means ZrO2 phase stabilized the copper, preventing crystallite growth. N2O results and TEM images exhibited that ZrO2 enhanced Cu dispersion and Cu particle size was almost under 5 nm. TGA result suggests that the suitable calcination temperature is above 650 K. In TPR patterns, CuO reduction temperature was decreased by ZrO2, and this phenomenon was correlated to XRD. We tested the catalysts activity for various parameters such as promoter loading, calcination temperature, feed ratio and reaction temperature. Zirconium oxide was believed to enhance the activity of catalyst and the best operation parameters to optimize catalyst’s performance are calcination temperature 673 K; O2/CH3OH feed ratio 0.3 and reaction temperature 523 K.
Appears in Collections:	[National Central University Department of Chemical & Materials Engineering] Electronic Thesis & Dissertation

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