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| DC 欄位 | 值 | 語言 |
|---|---|---|
| dc.contributor.advisor | 吳嘉文 | |
| dc.contributor.author | Jyun-Yi Yeh | en |
| dc.contributor.author | 葉俊毅 | zh_TW |
| dc.date.accessioned | 2021-06-17T03:21:57Z | - |
| dc.date.available | 2018-06-29 | |
| dc.date.copyright | 2018-06-29 | |
| dc.date.issued | 2018 | |
| dc.date.submitted | 2018-06-20 | |
| dc.identifier.citation | 1 Ruppert, A. M., Weinberg, K. & Palkovits, R. Hydrogenolysis Goes Bio: From Carbohydrates and Sugar Alcohols to Platform Chemicals. Angew. Chem.-Int. Edit. 51, 2564-2601.
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| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/69637 | - |
| dc.description.abstract | 1,5-戊二醇為合成高價值聚合物之重要單體，一般經由石油來源合成。但石油來源中缺乏五碳化合物，因此1,5-戊二醇實為工業合成程序中之副產物，進而使得全球的年產量相當低 (3000噸/年)。然而，隨著新聚合物的開發，1,5-戊二醇的需求量逐年成長，造就了1,5-戊二醇的高單價。因此，自生物質轉換所得之糠醛生產1,5-戊二醇的反應開發逐漸受到重視。 近年來，許多固體觸媒被成功應用於轉換糠醛至1,5-戊二醇，但皆須使用高壓氫氣搭配高溫的反應條件，如此嚴苛之反應環境導致製程耗能與不易控制等問題。本研究成功開發能於溫和條件下，生產75%高產率之1,5-戊二醇反應，其觸媒為金屬有機框架衍生氧化鋁支撐式白金觸媒，並搭配硼氫化鈉於水相環境中轉換糠醛為1,5-戊二醇。此反應之路徑分為兩步驟，糠醛先被氫化為糠醇，糠醇之呋喃環直接行開環反應，開環後之反應中間體再緊接著被氫化成為1,5-戊二醇。其中，硼氫化鈉不僅僅只扮演氫源之角色，其水解產物之衍生產物硼酸能協助開環反應步驟之進行。 | zh_TW |
| dc.description.abstract | 1,5-Petanediol (1,5-PD) is an essential chemical for industrial production of polymer and is mainly derived from petroleum. Unfortunately, 1,5-pentanediol is a side product in petroleum process. Thus, the worldwide capacity is low, and with increasing demand, the price of 1,5-pentanediol rises. In order to enhance higher capacity, the synthesis of 1,5-pentanediol through biomass process. In the biomass process, 1,5-pentanediol is converted from furfural through the ring-opening hydrogenation process which requires severe conditions leading to large energy consumption and system-controlling difficulties. Therefore, we develop a metal organic framework derived alumina supported platinum catalyst which enhances an ability to convert furfural into 1,5-pentanediol with high yield (75%) under mild condition assisted by sodium borohydride. The reaction pathway is proved that the furan ring of the furfuryl alcohol, hydrogenation product of furfural, is firstly open and hydrogenated into 1,5-pentanediol. The role of sodium borohydride is not just a hydrogen source but also an origin of the boric acid, a helping reagent of ring-opening step. | en |
| dc.description.provenance | Made available in DSpace on 2021-06-17T03:21:57Z (GMT). No. of bitstreams: 1 ntu-107-R05524079-1.pdf: 9591239 bytes, checksum: 494084f14febd89d944d5266aede957e (MD5) Previous issue date: 2018 | en |
| dc.description.tableofcontents | Table of Content
ABSTRACT i 摘要 ii Table of Content iii List of Figures v List of Tables vii 1. Introduction 1 1.1. Furfural 1 1.2. 1,5-Pentanediol 2 1.3. Liquid hydrogen source: chemical hydrides 8 1.4. Synthesis of Supported Catalyst 10 1.4.1. Immobilization of Catalyst 11 1.4.2. Metal organic framework 14 2. Objectives 19 3. Experimental 20 3.1. Chemicals and materials 20 3.2. Preparation of catalysts 25 3.2.1. Room temperature synthesis of MIL53-NH2 (Al) 25 3.2.2. Synthesis of Pt embedded MIL53-NH2 (MIL53-NH2 (Y-Pt, Al)) 26 3.2.3. MOF derived catalyst by calcination (Y-Pt@Al2O3-X) 27 3.2.4. Commercialized metal oxide, metal sulfide and carbon supported noble metal catalysts 28 3.3. Furfural to 1,5-pentandiol reaction 29 3.4. Characterization 30 3.4.1. Characterization of products 30 3.4.2. X-ray diffractometer (XRD) 31 3.4.3. Scanning electron microscope (SEM) 31 3.4.4. Energy dispersive spectroscopy (EDS) 31 3.4.5. Inductively Coupled Plasma-Mass Spectrometer (ICP/MS) 31 3.4.6. X-ray Photoelectron Spectroscopy (XPS) 32 3.4.7. Fourier Transform Infrared Spectrometer (FTIR) 32 3.4.8. Specific Surface Area & Pore Size Distribution Analyzer 32 3.4.9. Thermogravimetry/differential thermal analysis thermoanalyzer (TG-DTA) 33 3.5. Purification 33 4. Results and Discussions 35 4.1. Materials Characterizations 35 4.1.1. Properties of MIL53-NH2 (Y-Pt, Al) 35 4.1.2 Properties of Y-Pt@Al2O3-X 40 4.1.2.1. The effect of Pt precursor (K2PtCl4) using 40 4.1.2.2. The effect of Pt loading 42 4.1.2.3. The effect of calcination temperature 46 4.2. Furfural to 1,5-PD reaction 47 4.2.1. Blank test 47 4.2.2. Reaction optimization of commercial support catalyst 48 4.2.2.1. Noble metal effect 49 4.2.2.2. The effect of support 50 4.2.2.3. The effect of the hydrogen source 52 4.2.2.4. The effect of reaction temperature 53 4.2.2.5. The effect of the molar ratio of FA/sodium borohydride 55 4.2.2.6. The effect of the water volume 56 4.2.3. Reaction optimization of Y-Pt@Al2O3-X 57 4.2.3.1. The reaction temperature effect 57 4.2.3.2. The effect of the molar ratio of FA/sodium borohydride 58 4.2.3.3. The reaction time effect 60 4.2.3.4. The calcination temperature effect 61 4.2.4. Catalysts performance of commercial support platinum catalyst and the MOF derived platinum material. 62 4.2.5. Reaction mechanism studies 66 4.2.5.1. Reaction pathway studies 66 4.2.5.2. Activation energy calculation 68 4.2.5.3. Proposed mechanism 72 4.2.6. Purification 83 5. Conclusion 86 6. Future Prospect 87 7. Reference 88 Appendix 94 XPS pattern of different catalyst 94 | |
| dc.language.iso | en | |
| dc.subject | 糠醛 | zh_TW |
| dc.subject | 有機金屬框架衍生複合物 | zh_TW |
| dc.subject | 白金 | zh_TW |
| dc.subject | 硼氫化鈉 | zh_TW |
| dc.subject | 氧化鋁 | zh_TW |
| dc.subject | 有機金屬框架 | zh_TW |
| dc.subject | 溫和條件 | zh_TW |
| dc.subject | 5-戊二醇 | zh_TW |
| dc.subject | furfural | en |
| dc.subject | platinum | en |
| dc.subject | aluminum oxide | en |
| dc.subject | metal organic frameworks | en |
| dc.subject | mild condition | en |
| dc.subject | sodium borohydride | en |
| dc.subject | MOF-derived composites | en |
| dc.subject | 5-pentanediol | en |
| dc.title | "同步合成含鉑金屬有機框架(MIL-53(Al)-NH2)衍生鉑/氧化鋁複合物之高效率觸媒應用於硼氫化鈉輔助溫和條件轉化糠醛至1,5-戊二醇反應" | zh_TW |
| dc.title | De novo synthesis Pt-embedded MIL-53(Al)-NH2 derived Pt@Al2O3 composites for efficient furfural to 1,5-pentanediol conversion with assistance of NaBH4 | en |
| dc.type | Thesis | |
| dc.date.schoolyear | 106-2 | |
| dc.description.degree | 碩士 | |
| dc.contributor.oralexamcommittee | 鍾博文,陳文華,林裕川,汪進忠 | |
| dc.subject.keyword | 1,5-戊二醇,糠醛,硼氫化鈉,溫和條件,有機金屬框架,氧化鋁,白金,有機金屬框架衍生複合物, | zh_TW |
| dc.subject.keyword | 1,5-pentanediol,furfural,sodium borohydride,mild condition,metal organic frameworks,aluminum oxide,platinum,MOF-derived composites, | en |
| dc.relation.page | 98 | |
| dc.identifier.doi | 10.6342/NTU201801005 | |
| dc.rights.note | 有償授權 | |
| dc.date.accepted | 2018-06-21 | |
| dc.contributor.author-college | 工學院 | zh_TW |
| dc.contributor.author-dept | 化學工程學研究所 | zh_TW |
| 顯示於系所單位： | 化學工程學系 | |
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