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研究生: 吳岱恩
Dai-En Wu
論文名稱: 鈷的氧化價數對CoOx和Au/CoOx催化CO氧化活性的影響
Effect of Oxidation State of Cobalt Oxides on Their Catalytic Activity towards Oxidation of Carbon Mono-oxide
指導教授: 葉君棣
口試委員:
學位類別: 碩士
Master
系所名稱: 理學院 - 化學系
Department of Chemistry
論文出版年: 2000
畢業學年度: 88
語文別: 中文
論文頁數: 56
中文關鍵詞: 鈷的氧化價數CO氧化Au/Co3O4CoOx
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  • 本研究改變CoOx和Au/CoOx樣品中鈷的氧化價數(x = 1.00 ~ 1.33),並將樣品於固定床反應系統中測試其CO氧化的催化活性,以探討鈷的氧化價數對其催化活性的影響。在研究中使用TPR技術來定量樣品中氧原子的化學計量值,和利用XRD、TG/DTA、BET以及AA等方法來鑑定樣品的物理特性。
    CoOx樣品催化CO氧化所需的反應溫度和活化能,都會隨著樣品中氧原子化學計量值的增加而降低,而在Au/CoOx樣品上也具有相同的活性結果。從TG和TPR的結果中推證,在CoOx和Au/CoOx樣品進行催化反應時,樣品上會具有兩種能催化CO氧化的氧,其中活性較高的是Co3O4擔體上高活性的晶格氧離子,而活性較低的是吸附在CoOx表面上的氧分子。

    當金粒子支撐在Co3O4擔體上時,會在樣品上產生新的吸附位置。此吸附位置能增進樣品吸附CO的能力,而促進樣品在室溫下的催化活性。


    Catalysts of CoOx and Au/CoOx (x is a stoichiometry between 1.00 and 1.33) were prepared to study their catalytic activity towards the CO oxidation. The oxidation state of cobalt ions in these catalysts was evaluated with TPR (the temperature programmed reduction) technique. TPR reduction of CoOx samples was found to proceed through two resolvable steps, i.e., CoOx into CoO at 570 K and CoO to metallic Co at 640 K. The relative area observed for these two peaks in TPR traces was used to determine the stoichiometry x in freshly prepared catalysts. Their catalytic activities were tested in a fixed bed flow reactor.
    Measured activity generally increased with the stoichiometry x in catalysts of CoOx and Au/CoOx. The variation in activity was interpreted with an oxidation of CO by two kinds of oxygen species, i.e., oxygen molecularly adsorbed on CoOx surface and active oxygen ions in the lattice of Co3O4 spinel structures.

    An impregnation of Au particles on the surface of CoOx significantly enhances its catalytic activity. The promotion comes from an effective adsorption of CO on the interface between the particles and the surface.

    第一章 緒論 1-1 CO的毒性和消除 1-2 金觸媒催化CO氧化的活性 1-3 研究目的和方向 第二章 實驗方法 2-1 樣品的製備 2-1.1 Au/Co3O4樣品的製備 2-1.2 改變樣品中鈷的氧化價數 2-2 樣品的特性鑑定 2-2.1 BET表面積測定 2-2.2 X光粉末繞射 2-2.3 原子吸收光譜儀 2-2.4 熱分析儀 2-2.5 程溫還原系統 2-3 樣品催化活性測試 2-3.1 活性系統 2-3.2 圖譜分析 第三章 結果與討論 3-1 CoOx樣品的製備和其特性分析 3-1.1 Co3O4和CoO樣品的製備 3-1.2 Co3O4和CoO樣品的特性分析 3-1.3 Co3O4的程溫還原 3-2 催化CO氧化活性的測試 3-2.1 CoOx樣品的活性 3-2.2 Au/CoOx樣品的活性 3-3 CO的氧化機制 3-3.1 CoOx樣品催化CO氧化的機制 3-3.2 Au/CoOx樣品催化CO氧化的機制 第四章 結論 第五章 參考文獻

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