三相泥浆式反应器Three.ppt

* 例如以La1-xSrxBO3 (B = Mn, Fe, Co, Ni) 催化 NO和CO之反應，CO會先跟氧化態的觸媒反應生成CO2， 觸媒本身變為還原態；接著，NO會將還原態的觸媒氧 化成氧化態，NO則轉化成N2；如此循環不已。 酵素反應也有相同的例子。 尾語 固體觸媒催化反應之研究，從簡單的反應實驗到觸媒表面現象的鑑定與量測，使用的設備，由最簡單的微分型反應器或批式反應器到龐大且價昂的同步輻射器。涉及之範圍寬廣，事項繁雜。本短文僅就一般研究固體觸媒催化反應之方法與步驟簡單的介紹。因時間匆促，難免有疏漏，敬請惠予斧正。 * Jiang, B.S. (江秉勳), Chang, R. (張 睿),?Lin, Y.-C.*?Partial oxidation of ethanol to acetaldehyde over LaMnO3-based perovskites - A kinetic study.?Ind. Eng. Chem. Res.??2013; 52, 37-42.??/doi/abs/10.1021/ie300348u * Introduction Perovskite is a crystal structure with a ABO3 It possesses unique redox chemistry and oxygen mobility for versatile catalytic applications C.-L. Li, Y.-C. Lin. Applied Catalysis B: Environmental 107 (2011) 284 – 293 A: La, B: Mn or precious metal * Background:the redox cycle of ethanol partial oxiduction * XRD * TPR LaMnO3+xH2→LaMnO3-x+xH2O Mn4+→Mn3+ 755 777 Mn3+→Mn2+ B. Levasseur, S. Kaliaguine. Applied Catalysis A: General 343 (2008) 29–38 * Conversion * Carbon Atom Selectivity * Mars van Krevelen redox cycle - 1 Ethanol adsorption Oxygen adsorption Acetaldehyde desorption Water desorption Surface reaction * Ethanol adsorption: Oxygen adsorption: Surface reaction: Acetaldehyde desorption: Water desorption: Mars van Krevelen redox cycle - 2 * assume surface reaction as rate determining step assume oxygen adsorption as rate determining step assume ethanol adsorption as rate determining step assume acetaldehyde desorption as rate determining step assume water desorption as rate determining step * Nonlinear Regression * Determine The Rate Determining Step Residual sum of squares 反應速率方程式 LaMn LaMnPd Ethanol adsorption 0.0657502 0.230754 Oxygen adsorption 0.00361 0.006037311 Surface reaction 0.003771 0.006082438 Acetaldehyde desorption 0.026837 0.048336535 Water desorption 0.023958 0.048336535 * Surface Reaction Oxygen Adsorption LaMn rsurf T(K) ksurf Kad,1 Kad,2 523 134.1 7891.6 0.9 493 68.0 7894.8 1.7 473 33.0 7896.8 3.3 443 18.2 7896.8 5.4 LaMn roxi T(K) kad,