Cu/CexZr1-xO2觸媒進行甲苯完全氧化反應之研究; Complete oxidation of toluene by Cu/Ce1-xZrxO2

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Title:	Cu/CexZr1-xO2觸媒進行甲苯完全氧化反應之研究;Complete oxidation of toluene by Cu/Ce1-xZrxO2
Authors:	簡崇訓;Chong-Syun Jian
Contributors:	化學工程與材料工程研究所
Keywords:	鈰;銅;鋯;甲苯完全氧化;Toluene oxidation;Cu;CeO2;ZrO2
Date:	2009-06-30
Issue Date:	2009-09-21 12:31:41 (UTC+8)
Publisher:	國立中央大學圖書館
Abstract:	本研究使用Cu/CexZr1-xO2進行甲苯完全氧化反應，控制不同的製備條件來探討擔體中添加Zr所造成的影響。CexZr1-xO2擔體分別使用共沉澱法(CP)與初濕含浸法(IMP)製備，再將Cu依照不同比例負載至擔體表面。由反應結果顯示，Cu/CeO2觸媒銅擔載量以5%~7%活性最好，在250℃將甲苯完全氧化，過量擔載會使銅顆粒聚集不利活性。以共沉澱法製備的擔體觸媒，添加Zr會使活性下降；使用初濕含浸法製備的擔體觸媒，在Zr含量<20%活性獲得提升，但過量添加仍然會使活性變差。比較兩種製備法，在Zr<20%的情況下活性大小為：Cu/CexZr1-xO2 (IMP)>Cu/CeO2>Cu/CexZr1-xO2(CP)。由XPS以及H2-TPR的結果發現，在表面形成少量的CeO2-ZrO2結構能夠提高觸媒中Cu+所佔的比例，提供反應物更多的吸附位置，使觸媒活性提升。而CeO2-ZrO2結構必須經過500℃鍛燒8 hr 才能夠形成。本研究製備的觸媒中，5% Cu/Ce0.8Zr0.2O2 (500℃,8hr)表現出最佳的活性，能在230℃將甲苯完全氧化，且通過100 hr的耐久性測試後活性並沒有明顯衰退。 Cu/CexZr1-xO2 was used as catalyst for toluene total oxidation. Catalyst support was prepared by co-precipitation (CP) or impregnation (IMP), and copper was impregnated on the support with different weight percent. Cu loading amount between 5~7 wt.% show the highest activity, catalytic activity decreased when the copper amount increased. For CP support catalysts, Zr incorporation decreased the activity. For IMP support catalysts, adding ZrO2 on CeO2 (less than 20 molar％) improved catalytic activity. When X<0.2, the trend of decreasing activity was Cu/Ce-Zr(IMP)>Cu/CeO2>Cu/Ce-Zr(CP). Calcination temperature effect was studied for Zr free catalysts and Zr<20 molar%. For catalysts without Zr, lower calcination temperature showed better activity. For catalysts with Zr<20 molar%, the catalysts calcined at 500℃ showed better activity than those calcined at 300℃. Calcination time effect was also discussed. Catalysts calcined at 500℃, for 4 hours and 8 hours showed different results. For 8 hours calcination, catalysts with Zr<20 molar% showed better activity than Cu/CeO2. For 4 hours calcination, the catalyst adding Zr did not improve activity. From XPS and H2-TPR results, Zr impregnation on CeO2 surface increased Cu+ amount. Cu+ was the adsorption position of toluene, increasing Cu+ amount improves catalysts activity.
Appears in Collections:	[National Central University Department of Chemical & Materials Engineering] Electronic Thesis & Dissertation

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