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研究生: 李昆展
Kun-Chan Lee
論文名稱: 以稻殼灰分初濕含浸製備擔體銅觸媒之研究
指導教授: 張奉文
Feg-Wen Chang
口試委員:
學位類別: 碩士
Master
系所名稱: 工學院 - 化學工程與材料工程學系
Department of Chemical & Materials Engineering
畢業學年度: 89
語文別: 中文
論文頁數: 90
中文關鍵詞: 乙醇脫氫銅觸媒稻殼灰分活性
外文關鍵詞: dehydrogenation of C2H5OH, copper catalyst, rice husk ash, activity
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  • 本研究以初濕含浸法製備稻殼灰分擔載銅觸媒,實驗結果顯示:降低金屬載量,將有助於提升觸媒的分散度;觸媒的還原溫度隨載量增加而降低,但金屬粒徑卻隨載量增加而變大。
    Cu/SiO2-RHA觸媒應用在533K∼613K乙醇脫氫反應活性測試,結果顯示稻殼灰分擔體銅觸媒在反應溫度範圍內,僅有脫氫反應的發生,生成單一產物乙醛,且催化活性隨著反應溫度與金屬載量的增加而逐漸增高。
    本實驗採用5wt. %的Cu/SiO2-RHA觸媒,先經過723K下鍛燒3小時後,在573K的還原程序下還原1小時,及在613K下進行乙醇脫氫反應,可得到良好的催化活性,使得乙醇轉化率提升。
    經由TPR及N2O-titration的分析證明,稻殼灰分特有的擔體性質,使其呈現與金屬間較強的擔體效應,優於氧化矽膠擔體銅觸媒及氧化鋅擔體銅觸媒,是一種具有高促進效果的乙醇脫氫反應銅觸媒擔體。


    Rice husk ash (RHA) supported copper catalysts were prepared by impregnation method. During the investigations of preparation conditions, effects of copper loading, reduction temperature, reaction time and reaction temperature on catalytic behavior were presented and discussed. The results indicate that the metal dispersion increases with decreasing of copper loading; the reduction temperature decreases with increasing of copper loading, and the metal grain size increases with increasing of copper loading.
    RHA supported copper catalyst was examined in the dehydrogenation of C2H5OH at 533∼613K and it formed a single product C2H4O. The results also indicate that the catalytic activity increases with increasing of reaction temperature and copper loading; the activity of copper catalyst achieves a maximum value with a copper loading of 5 wt.% , calcined at 723K for 3h and reduced at 573K for 1h in C2H5OH dehydrogenation at 613K.
    Moreover, RHA is found to be preferable over silica gel and ZnO as a catalyst support as revealed by the TPR and N2O titration techniques.

    內容 頁數 中文摘要 …………………………………………………………....I 英文摘要 …………………………………………………………...II 目錄 ………………………………………………………………..III 圖索引 …………………………………………………………….…...V 表索引 …………………………………………………...………..VIII 第一章 緒論…………………………………………………………...1 第二章 文獻回顧……………………………………………………...6 2-1 稻殼灰分的製備程序………………………………….……......6 2-2 含浸法製備擔體銅觸媒…………………………………........11 2-3 擔體效應…………………………………………………........15 2-4 乙醇脫氫反應……………………………………………........16 第三章 實驗方法與裝置…………………………………………...20 3-1 觸媒擔體的製備與分析…………………………………....20 3-1-1 觸媒擔體的製備─稻殼前處理………………………….......20 3-1-2 擔體的分析……………………………………………….......25 3-2 Cu/SiO2-RHA觸媒的製備………………………………........31 3-3 觸媒的鑑定分析………………………………………........32 3-3-1 熱重分析(TGA)、XRD、SEM及TEM分析………............32 3-3-2 程溫還原(TPR)……………………………………….......33 3-3-3 銅觸媒表面積測量……………………………………........35 3-4 觸媒的活性測試─乙醇脫氫反應……………………........37 3-5 實驗流程與操作變數…………………………………........39 3-6 數據的計算與實例……………………………………........41 3-7 儀器及藥品……………………………………………........45 第四章 結果與討論……………………………………………...48 4-1 Cu/SiO2-RHA觸媒製備條件的探討………………….....48 4-1-1 不純物的分析…………………………………………...48 4-1-2 觸媒還原程序的探討…………………………………...48 4-1-3 金屬載量對觸媒活性的影響…………………………...58 4-1-4 反應時間的選擇………………………………………...64 4-1-5 反應溫度對於乙醇脫氫反應的影響…………………...67 4-2 觸媒製備方法及擔體效應的反應活性比較………….......69 第五章 結論……………………………………………………..80 參考文獻 …………………………………………………………...82 附錄 實驗數據………………………………………………...88

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