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Preparation of Copper/Samarium Oxide-Cerium Oxide Catalyst for Steam Reforming of Methanol
Wang, Hsiang -Ping
|關鍵字:||steam reforming of methanol;甲醇蒸汽重組;oxygen-iron-conducting material;nanocatalyst;hydrogen;導氧離子材料;奈米觸媒;氫氣||出版社:||化學工程學系所||引用:|| 燃料電池論文集，台灣電力公司  燃料電池之特性與運用，行政院國家科學委員會科學技術資料中心  官荻偉，探討顆粒性厭氧產氫反應槽中各微生物組成關係對產氫效能的影響，國立中興大學環境工程學系碩士學位論文(2007)  張立德，奈米材料，五南圖書股份有限公司出版  牟季美，張立德，奈米材料和奈米結構，滄海書局  B. Lindström, and L. J. Pettersson, "Hydrogen generation by steam reforming of methanol over copper-based catalysts for fuel cell applications", International Journal of Hydrogen Energy, 26 (2001) 923–933  G. Mul, and A. S. Hirschon, "Effect of preparation procedures on the activity of supported palladium/lanthanum methanol decomposition catalysts", Catalysis Today, 65 (2001) 69-75  M. Wang, K. Do. Woo, and D. K. Kim, "Preparation of Pt nanoparticles on carbon nanotubes by hydrothermal method", Energy Conversion and Management, 47 (2006) 3235–3240  C.K. Lambert, and R.D. Gonzalez, "Rh/SiO2 catalysts prepared by the sol-gel method", Microporous Materials 12 (1997) 179-188  A. Vazquez, T. Lopez, R. 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Ayabe, "Hydrogen production by oxidative methanol reforming on Pd/ZnO", Applied Catalysis A：General 283(2005) 125-135  S. Liu, K. Takahashi, K. Fuchigami, and K. Uematsu, "Hydrogen production by oxidative methanol reforming on Pd/ZnO：Catalyst deactivation", Applied Catalysis A：General 299 (2006) 58-65  S. Liu, K. Takahashi, H. Eguchi, and K. Uematsu, "Hydrogen production by oxidative methanol reforming on Pd/ZnO：Catalyst preparation and supporting materials", Catalysis Today 129 (2007) 287-292  李志甫, X-射線法, 高立圖書有限公司  王亦凱, 邱宏明, 李秉傑, 非均勻系催化原理與應用, 國立編譯館  http://www.hk-phy.org/atomic_world/tem/tem02_c.html  http://www.chemedu.ch.ntu.edu.tw/lecture1/GC.htm  T. D. Nguyen, D. Mrabet, and T. O. Do, "Controlled Self-Assembly of Sm2O3 Nanoparticles into Nanorods：Simple and Large Scale Synthesis using Bulk Sm2O3 Powders", J. Phys. Chem. C 2008, 112, 15226-15235  葉怡成，實驗計劃法—製程與產品最佳化，五南圖書股份有限公司  陳順與，鄭碧娥，實驗設計，華泰書局  J. Papavasiliou, G. Avgouropoulos, and T. Ioannides, "Effect of dopants on the performance of CuO-CeO2 catalysts in methanol steam reforming", Applied Catalysis B：Environmental 69 (2007) 226-234||摘要:||
In the thesis, the purpose of this study is to prepare nanocatalyst Cu supported on Sm2O3-CeO2 and to apply it on steam reforming of methanol. The parameters of catalyst preparation include the different amounts of Cu, ratio of samarium oxide to cerium oxide, temperature of calcinations, types of dispersant, amount of dispersant, method of mixing, amount of promoter, concentration of precursor. Operating conditions in steam reforming of methanol are molar ratio of H2O/CH3OH, weight hourly space velocity, and stability of catalysts.
The results show that the amount of copper at 25wt% has a higer activity than others. The ratios of samarium oxide to cerium oxide at 25wt% and 75wt% made the best hydrogen yield. Different calcination temperatures can influence the pore size of catalyst, and the temperature of calcination at 500℃ enhanced the hydrogen yield greatly. Adding the dispersant of 1-Hexadecyl trimethyl ammonium bromide can make the catalyst obtain large surface area and have high activities. The content of dispersant can influence the surface area and total pore size of the that using catalyst. The catalystic activity using method of ultrasound is better than ultrasound and stirring. Adding few ZnO as promoter to Cu/Sm2O3-CeO2, the hydrogen yield was obtained near 95% at 280℃. The concentrations of precursor at 0.007M and 0.005M made the particles more smaller, but the hydrogen production rate was lower than that at 0.01M.
The catalyst of [Cu(80)/ZnO(20)](25)/[Sm2O3(25)-CeO2(75)](75) was used to proceed the reaction of steam reforming of methanol. With 1.3 of molar ratio of water to methanol, the hydrogen yield was 95% and the hydrogen production rate was 110.3mmmol/s*kg.cat at 280℃. The best performance of the catalyst was at 7.7hr-1 of weight hourly space velocity. In 100-hour duration of test, the activity decreased about 63%, and CO2 selectivity still kept at above 96% after 100h of reaction.
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