Please use this identifier to cite or link to this item: http://hdl.handle.net/11455/3547
標題: 奈米級被擔持氧化鎢觸媒之甲醇氧化反應研究
Oxidation of Methanol over the Nanoscale Supported Tungsten Oxide Catalysts
作者: 鄭貴寧
Cheng, Kuei-Ning
關鍵字: nano-catalysts
奈米觸媒
metal oxide
methanol oxidation reaction
acid sites
redox sites
金屬氧化物
甲醇氧化反應
出版社: 化學工程學系所
引用: 1 R.Thomas, E.M.Ranoers, V.H.J.DeBeer, et al. “Characterization of γ-alumina-suppouted molybdenum oxide and tungsten oxide ; Reducibility of the oxidic state versus hydrodesulfurization activity of the sulfided state” Catal.1982,76:241-253. 2 C.B gey , L.Hilaire, L. Hilaire, G. Maire. “WO3-CeO2 and Pd/WO3 CeO2 as potential catalysts for reforming applications” J. Catal.2001,198:208-222. 3 C.B gey, L.Hilaire, G.Maire. “Catalysis on Pd/WO3 and Pd/WO2: effect of the modifications of the surface states due to redox treatments on the skeletal rearrangement of hydrocarbons” .J.Catal.1999,184:406-42. 4 李芳柏,古國榜,李新軍等“WO3/TiO2奈米材料的制備及光催化性能”物理化學報,2000,1611:997-1002 5 C.Martin, I. Martin .V. Rives, G. Solana. “Physicochemical characterization of WO3/ZrO2 and WO3/Nb2O5 catalysts and their photoactiveity for 4-nitrophenol photooxidation in aqueous dispersion”J.Mater.Science,1997,32:6039-6047 6 Mohit Badlani and Israel E. Wachs. “Methanol: “a smart chemical probe molecule” Catal. Lett.75 ,2001 7 W. P. Halperin, Rev. of Modern Phys., 58, 532, 1986. 8 P. Ball and L. Garwin. “Science at the atomic scale.” Nature, 355, 761-766, 1992. 9 王世敏、許祖勛及傅晶,“奈米材料製備技術”,化學工業出版社,北京,2001. 10 陳嘉銘,奈米鎂-鎳合金於加氫/脫氫反應的應用:PEG胺化反應及奈米碳管的成長,國立中興大學化學工程學系博士論文,2004. 11 林豐智及永山時男,日本化學會誌,6,1050,1984 12 余衛國及錢捷,“奈米材料在催化加氫反應中的應用與研究進展” 浙江化工,34,27-30,2003. 13 R. Raja, T. Khimyak, J. M. Thomas, S. Hermans, and B. F. G. Johnson. “Single-step, highly active, and highly selective nanoparticle catalysts for the hydrogenation of key organic compounds.” Angew. Chem. Int. Ed., 40(24), 4638-4642, 2001. 14 R. Raja, G. Sankar, S. Hermans, D. S. Shephard, S. Bromley, J. M. Thomas, and B. F. G. Johnson. “Preparation and characterization of a highly active bimetallic (Pd-Ru) nanoparticle heterogeneous catalyst.” Chem. Commun., 16, 1571-1572, 1999. 15 J. P. Wiloxn, T. R. Thuston, J. E. Martin. “Application of metal and semiconductor nanoclusters as thermal and photo-catalysis.” 95, Atlanta Airport Marriott. Atlanta, Georgia, U.S.A., 143, 1995. 16 O. Alexeev and B. C. Gates. “Iridium clusters supported on γ-Al2O3: Structural characterization and catalysis of toluene hydrogenation.” J. Catal., 176(2), 310-320, 1998. 17 N. E. Bogdanchikova, S. Fuentes, M. Avalos-Borja, M.; M. H. Far
摘要: 近年來由於奈米技術的發展,而使得觸媒有的新的發展方向,由於奈米粒子具有高表面積、高表面能、高表面結合能以及很高的化學活性的特性,故國際上已把奈米粒子催化劑稱為第四代催化劑。 本研究中以水熱法合成出奈米級高比表面積的γ-Al2O3、Nb2O5、TiO2、ZrO2、CeO2為觸媒擔體,分別擔持1、3、5、10、20% 氧化鎢金屬氧化物為活性相。以TEM、XRD、BET、ICP對其做特性分析,並運用拉曼(Raman)光譜對奈米級被擔持氧化物觸媒其做表面結構進行分析,以瞭解表面金屬氧化物之動態變化。並進行甲醇氧化反應以氣相層析儀分析產物濃度,而得知此奈米級被擔持氧化物觸媒對氧化反應之活性及選擇性。 甲醇氧化反應研究結果顯示WOx/Al2O3、WOx/Nb2O5 、WOx/TiO2、WOx/ZrO2具有酸性基位於觸媒表面上,而 WOx /CeO2只有氧化還原基位位於觸媒表面。歸納反應結果以WOx/Al2O3此系列的被擔持觸媒之轉化率最好,並發現在鎢的附載量為3%以及5%時,轉化率為最佳。
In recent years, the catalyst have the new developing direction due to the development of nanometer technology. Because nanometer particle can have characteristics including high surface area, high binding energy and very high chemical activation, so Nanoscale particle catalyst was called the fourth generation of catalyst internationally. Nanoscale supported metal oxide catalysts were synthesized by hydrothermal method. The supports are γ-Al2O3, Nb2O5, TiO2, ZrO2 and CeO2, and 1、3、5、10、20% of WO3 were deposited on the previous oxide supports, respectively. The physical properties and structural information were characterized by TEM, XRD, BET, ICP and in situ Raman spectroscopy. Raman results confirm that the desired molecular arrangements of the active surface metal oxide phases have been achieved. The reactivity/selectivity properties of the nano catalysts are chemically probed with steady-state catalytic studies of propane oxidative dehydrogenation and methanol oxidation reactions. The results of methanol oxidation reaction reveal that there are acid sites on the surface of WOx/Al2O3 , WOx/Nb2O5 , WOx/TiO2 and WOx/ZrO2, and WOx / CeO2 only have redox sites on the surface of the other catalysts. To sum up the reaction result, the conversion of WOx/Al2O3 catalyst was the best. Simultaneously it was found that when loading of tung 3% and 5% , conversion ratio were the best.
URI: http://hdl.handle.net/11455/3547
其他識別: U0005-0311200616191400
文章連結: http://www.airitilibrary.com/Publication/alDetailedMesh1?DocID=U0005-0311200616191400
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