Cu/CexZr1-xO2觸媒進行甲苯完全氧化反應之研究｜國立中央大學博碩士論文系統

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研究生：	簡崇訓 Chong-Syun Jian
論文名稱：	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
指導教授：	楊思明 Sze-Ming Yang
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：	97
語文別：	中文
論文頁數：	71
中文關鍵詞：	鈰、銅、鋯、甲苯完全氧化
外文關鍵詞：	Toluene oxidation, Cu, CeO2, ZrO2
相關次數：	點閱：10 下載：0
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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.

摘  要	I
Abstract	II
目  錄	IV
圖 目 錄	V
表 目 錄	VII
第一章 緒論	1
第二章  文獻回顧	2
2.1銅觸媒催化反應	2
2.1.1 CuO觸媒	2
2.1.2 CeO2擔體	3
2.1.3 CexZr1-xO2結構與氧化還原特性	3
2.2 Cu/CeO2觸媒進行CO氧化反應	5
2.3甲苯完全轉化反應	7
2.4觸媒製備方式的影響	10
第三章  實 驗	13
3.1實驗藥品	13
3.2 實驗儀器	14
3.3實驗方法	15
3.3.1觸媒擔體CeXZr1-XO2製備	15
3.3.2銅觸媒製備(初濕含浸法)	16
3.3.3進料濃度計算	17
3.3.3反應活性測試	17
3.4 鑑定方法	19
第四章 結果與討論	23
4.1 X光繞射譜圖(XRD)	23
4-2 觸媒TEM影像	28
4-3 觸媒表面積及元素分析	31
4.4 觸媒表面化學分析(XPS)	33
4-5 H2-TPR	48
4.6觸媒反應結果	49
第五章 結論	58
參 考 文 獻	60

                                

[1] Y. Ono, M. Shibata, T. Inui, J. Mol. Catal. A-Chem. 153 (2000) 53-62.
[2] C.Y. Shiau, M.W. Ma, C.S. Chuang, Applied Catalysis a-General 301 (2006) 89-95.
[3] G. Avgouropoulos, T. Ioannides, H.K. Matralis, J. Batista, S. Hocevar, Catalysis Letters 73 (2001) 33-40.
[4] G. Avgouropoulos, T. Ioannides, C. Papadopoulou, J. Batista, S. Hocevar, H.K. Matralis, Catalysis Today 75 (2002) 154-167.
[5] K.C. Talor, Rev.-Sci. Eng. 35 (1993).
[6] P. Fornasiero, R. Dimonte, G.R. Rao, J. Kaspar, S. Meriani, A. Trovarelli, M. Graziani, Journal of Catalysis 151 (1995) 168-177.
[7] G. Vlaic, R. Di Monte, P. Fornasiero, E. Fonda, J. Kaspar, M. Graziani, Journal of Catalysis 182 (1999) 378-389.
[8] K. Otsuka, Y. Wang, M. Nakamura, Applied Catalysis a-General 183 (1999) 317-324.
[9] P. Pantu, K. Kim, G.R. Gavalas, Applied Catalysis a-General 193 (2000) 203-214.
[10] C. Descorme, Y. Madier, D. Duprez, Journal of Catalysis 196 (2000) 167-173.
[11] W. Liu, M. Flytzani-Stephanopoulos, Journal of Catalysis 153 (1995) 317-332.
[12] B. Skarman, D. Grandjean, R.E. Benfield, A. Hinz, A. Andersson, L.R. Wallenberg, Journal of Catalysis 211 (2002) 119-133.
[13] S. Minico, S. Scire, C. Crisafulli, S. Galvagno, Applied Catalysis B-Environmental 34 (2001) 277-285.
[14] D. Andreeva, V. Idakiev, T. Tabakova, A. Andreev, R. Giovanoli, Applied Catalysis a-General 134 (1996) 275-283.
[15] S.C. Kim, C.Y. Park, Res. Cme. Intermed 28 5 (2002), 441-449.
[16] C.H. Wang, S.S. Lin, C.L. Chen, H.S. Weng, Chemosphere 64 (2006) 503-509.
[17] M.F. Ribeiro, J.M. Silva, S. Brimaud, A.P. Antunes, E.R. Silva, A. Fernandes, P. Magnoux, D.M. Murphy, Applied Catalysis B-Environmental, 70 (2007), 384-392.
[18] H.L. Tidahy, S. Siffert, F. Wyrwalski, J.F. Lamonier, A. Aboukais, Catalysis Today, 199 (2007), 317-320.
[19] M.F. Luo, M. He, Y.L. Xie, P. Fang, L.Y. Jin, Applied Catalysis B-Environmental 69 (2007) 213-218.
[20] 吳宗昆，「於陶瓷纖維紙上合成Au/CeO2 並進行苯及甲苯的完全氧化反應之研究」，國立中央大學化學工程與材料工程研究所碩士論文，2007年。
[21] J.C.S. Wu, T.Y. Chang, Catalysis Today 44(1998) 111-118.
[22] J.C.S. Wu, Z.A. Lin, F.M. Tsai, J.W. Pan, Catalysis Today 63(2000) 419-426.
[23] A.K.C. F.T. Saad, chemosphere 38 (1999) 2109.
[24] C.Q. Hu, Q.S. Zhu, Z. Jiang, Y.Y. Zhang, Y. Wang, Microporous and Mesoporous Materials 113 (2008) 427-434.
[25] D. Delimaris, T. Ioannides, Applied Catalysis B-Environmental 89 (2009) 295-302.
[26] P. Zimmer, A. Tschope, R. Birringer, Journal of Catalysis 205 (2002) 339-345.
[27] J.F. Moulder, W.F. Stickle, P.E. Sobol, K.D. Bomben, Physical Electronics, Inc (1992).
[28] G. Avgouropoulos, T. Ioannides, Applied Catalysis a-General 244 (2003) 155-167.
[29] W. Liu, M. Flytzani-Stephanopoulos, Chemical Engineering Journal 64 (1996) 283-294.
[30] L. Dong, Y. Hu, M. Shen, T. Jin, J. Wang, W. Ding, Y. Chen, Chemistry of Materials 13 (2001) 4227-4232.
[31] W. Liu, M. Flytzani-Stephanopoulos, Journal of Catalysis 153 (1995) 317-332.
[32] C.C. Chusuei, M.A. Brookshier, D.W. Goodman, Langmuir 15 (1999) 2806-2808.

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