二氧化鋯觸媒之製備、修飾、鑑定及催化反應

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Title:	二氧化鋯觸媒之製備、修飾、鑑定及催化反應
Other Titles:	The Preparation, modification, Characterization and Catalytic Reaction of Zirconium Dioxide
Authors:	許雅珊 Hsu, Ya-Shan
Contributors:	柯安男 Ko, An-Nan 東海大學化學系
Keywords:	二氧化鋯;硫酸修飾之中孔型二氧化鋯;異丙醇;正丁醇 Zriconium dioxide;Sulfated mesoporous zirconium dioxide;isoporpanol;1-Butanol
Date:	2005
Issue Date:	2011-05-19T08:00:03Z (UTC)
Abstract:	本論文探討異丙醇與正丁醇之催化反應。使用二氧化鋯、硫酸修飾的二氧化鋯(ZrO2/S)以及硫酸修飾之中孔型二氧化鋯(meso-ZrO2/S)等三種作為觸媒。藉由X射線粉末繞射光譜、元素分析、感應偶合電漿-原子放射光譜、霍氏紅外線光譜、掃描式與穿透式電子顯微鏡、物理吸附、溫度程控脫附，鑑定觸媒組成結構、表面積、孔洞形狀與大小以及酸鹼量與強度等性質。發現觸媒於硫酸修飾前與後結構分別以單斜晶體與正方晶體型式為主。三種觸媒的表面積與酸量大小依序為：meso-ZrO2/S>ZrO2/S>ZrO2；而三種觸媒皆幾乎不具酸性。利用固定床流動反應器，於150~200℃及一大氣壓下分別進行異丙醇與正丁醇之催化反應。異丙醇脫水反應產物以丙烯為主，正丁醇脫水反應產物則以1-丁烯與2-丁烯異構物為主，且順-2-丁烯/反-2-丁烯比值接近1，顯示酸性觸媒之催化結果。而此兩反應催化活性依序為：meso-ZrO2/S>ZrO2/S>ZrO2，此結果與觸媒酸量及表面積呈現相同的順序。ZrO2/S觸媒催化異丙醇與正丁醇脫水反應的活化能分別為61.8與100.0kJ/mol，而meso-ZrO2/S觸媒在異丙醇與正丁醇脫水反應的活化能分別為45.1與76.1kJ/mol。 This thesis investigates the catalytic reactions of both isopropanol and 1-butanol. Zirconium dioxide, sulfuric acid modified zirconium dioxide (ZrO2/S), and sulfuric acid modified mesoporous zirconium dioxide (meso-ZrO2/S) were utilized as catalysts. These materials were characterized with X-ray powder diffraction, element analysis, induced coupled plasma-atomic emission, Fourier transform infrared spectroscopy, scanning and transmission microscopy, physisorption, and temperature -programmed desorption so as to obtain catalyst properties, i.e., composition, structure, surface area, pore shape and size, and the amount and strength of acid and base sites. The main structures of ZrO2 and sulfated ZrO2 are monoclinic and tetragonal, respectively. The sulface area and acid amount follow the decreasing order of meso-ZrO2/S>ZrO2/S>ZrO2. These catalysts own negligible basicity . The catalytic reactions of both isopropanol and 1-butanol were carried out at 150-200℃ and 1atm. With isopropanol, the main product is propylene. In the case of 1-butanol, 1-butene and isomers of 2-butene are the main products. In addition, the ratios of cis to trans-2-butene are close to 1, indicating catalysis via solid acids. For these two reactions, the catalytic activity decreases as follow：meso-ZrO2/S>ZrO2/S>ZrO2, in accordance with catalyst acid amount and surface area. In the reactions of both isopropanol and 1-butanol over ZrO2/S, the activation energies are 61.8 and 100.0 kJ/mol, respectively. With meso-ZrO2/S, the corresponding values are 45.1 and 76.1 kJ/mol.
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