指導教授:吳嘉文臺灣大學:化學工程學研究所吳霈恩Wu, Pei-EnPei-EnWu2014-11-252018-06-282014-11-252018-06-282014http://ntur.lib.ntu.edu.tw//handle/246246/261190由於能源的需求越來越大,加上石油的供應終將面臨短缺,有再生能力並且環保的生質能源因此受到矚目。其中,由木質纖維素所製備的2,5-二甲基呋喃因性質接近汽油,因此可取代汽油或成為汽油添加物。藉由氫化可以將5-甲基糠醛轉換成2,5-二甲基呋喃。氫化反應大多需要高溫達成活化能與通入高壓氫氣提高氫氣於溶劑中的溶解值。在此,我們提供一反應系統在室溫與室壓下即能製備2,5-二甲基呋喃。 此實驗由ZIF-67(Zeolitic Imidazolate Framework)合成的雙功能鈀鈷奈米孔洞碳材,鈀能提供氫化反應所需的金屬表面並利用鈷催化氫硼化鈉可於液態產氫。鈀與鈷在同一材料上的協同作用使得我們可以在室溫與室壓下得到83.07% 產率的2,5-二甲基呋喃。The ever increasing demand for energy combined with the diminishing supply of fossil fuel signals the need to search for an alternative energy source. 2,5-Dimethylfuran (DMF) is a green and renewable fuel due to its lignocellulosic origin. The production of DMF results from the hydrogenation and hydrogenolysis of 5-Hydroxymethylfurfural (HMF). Hydrogenation processes often require purging the system with high pressure hydrogen to increase the solubility of hydrogen in the solvent, all the while using high temperatures for the hydrogenation reactions to occur. Herein, we proposed a novel method in which DMF could be synthesized in high yields under atmospheric pressure and room temperature. A bifunctional Pd/CoNC material of ZIF-67 descent was synthesized in which Palladium provides a hydrogenation surface and Cobalt catalyzes the production of hydrogen from an aqueous source, Sodium Borohydride (NaBH4). The synergetic effects of Cobalt and Palladium on the same support helped achieve 83.07% DMF yields.1. INTRODUCTION 1 1.1. ENERGY CRISIS 1 1.2. BIOMASS DEVELOPMENT 4 1.3. BIOMASS CONVERSION 6 2. PAPER SURVEY 9 2.1. METAL ORGANIC FRAMEWORK (MOF) BASED CATALYSTS 9 2.2. INCIPIENT WETNESS IMPREGNATION37 11 2.3. PRODUCTION OF 2,5-DIMETHYLFURAN 15 3. OBJECTIVE 20 4. EXPERIMENTAL 22 4.1. CHEMICALS AND MATERIALS 22 4.2. EQUIPMENT 23 4.3. PROCEDURE FOR PRODUCTION OF 2,5-DIMETHYLFURAN 24 4.3.1. Batch Reactions 24 4.3.2. Semi-Batch Reactions 26 4.4. CATALYST SYNTHESIS 28 4.4.1. ZIF-67 Synthesis 28 4.4.2. ZIF-67 to Pd/CoNC Conversion 30 4.5. CHARACTERIZATION 31 4.5.1. Scanning Electron Microscope (SEM) 31 4.5.2. Transmission electron microscopy (TEM) 37 4.5.3. Specific Surface Area Analyzer 42 4.5.4. X-Ray Diffraction (XRD) 44 4.5.5. Thermogravimetric Analysis 46 4.5.6. Calibration Curve for DMF 48 4.5.7. Calibration Curve for MFAD 48 5. RESULTS AND DISCUSSION 49 5.1. HMF AS THE STARTING REACTANT 49 5.1.1. Effect of Catalyst Amount 49 5.1.2. Effect of Reaction Temperature 51 5.1.3. Effect of Reaction Time 51 5.1.4. Effect of NaOH addition 53 5.2. COMPARISON OF DIFFERENT STARTING REACTANTS 55 5.3. PALLADIUM AND COBALT ON SAME OR DIFFERENT SUPPORTS 57 5.4. REACTIONS STARTING WITH MFAD 58 5.4.1. With or Without Acid Addition 58 5.5. DIFFERENT STARTING REACTANTS UNDER OPTIMUM CONDITIONS 62 5.6. EFFECT OF ATM OR NON-ATM PRESSURE TESTS 63 5.7. SYNERGETIC EFFECTS OF COBALT AND PALLADIUM 64 6. CONCLUSION 66 7. FUTURE PROSPECTS 67 8. REFERENCE 693517226 bytesapplication/pdf論文公開時間:2017/08/14論文使用權限:同意無償授權生質能源2,5-二甲基呋喃ZIF-67氫化反應雙官能化[SDGs]SDG7利用液態氫源與雙功能鈀鈷的碳球在常溫常壓下製備2,5-二甲基呋喃Novel Synthesis of 2,5-Dimethylfuran under Ambient Conditions Utilizing ZIF-67 Derived Bifunctional Carbon Supported Palladium and Cobalt with Aqueous Hydrogen Sourcethesishttp://ntur.lib.ntu.edu.tw/bitstream/246246/261190/1/ntu-103-R01524095-1.pdf