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| DC 欄位 | 值 | 語言 |
|---|---|---|
| dc.contributor.advisor | 吳嘉文(Chia-Wen(Kevin) | |
| dc.contributor.author | Ying-Hui Chen | en |
| dc.contributor.author | 陳瀅惠 | zh_TW |
| dc.date.accessioned | 2021-06-17T03:21:00Z | - |
| dc.date.available | 2023-06-26 | |
| dc.date.copyright | 2018-06-26 | |
| dc.date.issued | 2018 | |
| dc.date.submitted | 2018-06-22 | |
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| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/69610 | - |
| dc.description.abstract | 傳統上在製備以金屬有機骨架為基材的擔體型觸媒時，通常是加入金屬粒子或金屬前驅物到已生成的金屬有機骨架中，因此現今在材料合成上，仍存在搭載量低以及金屬粒子聚集的限制。在本研究中，我們以原位合成法( de novo synthesis)，透過在最初同時加入觸媒金屬和金屬有機骨架之前驅物達到更充分地混合，並對後續金屬骨架生成和搭載觸媒金屬還原進行階段溫控，以更有效地藉由金屬有機骨架的形成來限制觸媒金屬粒子的生長。我們成功的合成了具有高度分散性的白金粒子於UiO-66-NH2骨架的粉粒及薄膜，藉由XRD, TEM, BET, ICP/MS等分析確認我們成功合成此材料。隨後，藉調控搭載白金量、生長時間以及苯甲酸加入量，找出此觸媒最佳化生長條件為: 白金與鋯加入莫耳比0.5，反應兩天，以及加入苯甲酸量41.4微莫耳。此產物的白金含量為16.5 wt.%，產物最終白金/鋯莫耳比為0.335，較大部分傳統手法合成的金屬有機骨架觸媒都高。在研究的最後，我們將原位合成法成功地拓展到具催化性薄膜的合成上，將其製備於氧化鋁圓片及氟化氧化錫玻璃板。此薄膜的厚度可達到1微米以下，並依需求製備出不同白金含量的薄膜，可望於未來有更廣泛地應用。 | zh_TW |
| dc.description.abstract | Although MOF-derived heterogeneous catalysts have been widely prepared by adding metal nanoparticles into pre-synthesized MOF or its precursors, there are still some problems such as the loading amount and uniformity of the metal. In this study, we load metal nanoparticles (i.e. Pt) into MOF (i.e. UiO-66-NH2) with controllable loading amount and uniformity through a de novo synthesis where metal and MOF precursors were added together in the very beginning. After careful optimization of temperature program of MOF structuring and metal reduction, we successfully prepare Pt-loaded UiO-66-NH2 (i.e. Pt@UiO-66-NH2) in the morphology of particles and films. The synthesized Pt@UiO-66-NH2 samples are characterized with XRD, TEM, BET, ICP/MS measurements. We optimize the Pt loading ratio, growth time, and amount of benzoic acid to be Pt/Zr=0.5, 48 h, and 41.1 mmol, respectively. The highest loading amount of Pt is 16.5 wt.% (i.e. Pt/Zr ratio is 0.335), which is much higher compared to previous studies. Finally, we expend this de novo synthesis for preparing Pt@UiO-66-NH2 on α-Al2O3 and FTO substrates, and Pt@UiO-66-NH2 with different Pt loadings and film thickness (less than 1 μm) can be prepared. We envision the prepared Pt@UiO-66-NH2 particles and films would have great potential in the catalytic applications. | en |
| dc.description.provenance | Made available in DSpace on 2021-06-17T03:21:00Z (GMT). No. of bitstreams: 1 ntu-107-R05524049-1.pdf: 10533517 bytes, checksum: a9cd3f0dfd70099023e46f7301bfc53b (MD5) Previous issue date: 2018 | en |
| dc.description.tableofcontents | 1. Introduction 1
1.1. Metal-Organic Frameworks (MOFs) 1 1.2. Heterogeneous MOF-derived catalysts 4 2. Literature review 12 2.1. Chemical vapor infiltration 14 2.2. Solid grinding 16 2.3. Incipient wetness impregnation 17 2.4. Impregnation 18 2.5. In situ synthesis 20 2.6. De novo synthesis 24 3. Objectives 33 4. Experimental 36 4.1. Chemicals and Materials 36 4.2. Equipment 37 4.3. Preparation of MOF and MOF-derived Heterogeneous Particles 38 4.3.1. Synthesis of UiO-66-NH2 Particles 38 4.3.2. De Novo Synthesis of Pt@ UiO-66-NH2 Particles 38 4.4. Fabrication of Pt@UiO-66-NH2 thin film on α-Al2O3 41 4.5. Fabrication of Pt@UiO-66-NH2 thin film on FTO 42 4.6. Characterizations 43 4.6.1. X-Ray Diffractometer (XRD) 43 4.6.2. Field-Emission Scanning Electron Microscope (FE-SEM) 43 4.6.3. SEM-Energy Dispersive Spectroscopy (EDS) 44 4.6.4. Transmission Electron Microscope (TEM) 44 4.6.5. TEM-Energy Dispersive Spectroscopy (EDS) 45 4.6.6. ICP/MS 45 4.6.7. X-ray Photoelectron Spectroscopy (XPS) 45 4.6.8. Specific Surface Area & Pore Size Distribution Analyzer by Gas Adsorption Method 46 5. Results and Discussion 47 5.1. Characterization of UiO-66-NH2 and Pt@UiO-66-NH2 particles 47 5.2. Effect of embedded platinum amount 52 5.3. Effect of Different Growth Time of Pt@UiO-66-NH2 Particles 63 5.4. Effect of amount of Benzoic Acid 71 5.5. Summary of Pt@UiO-66-NH2 Particle Preparation 79 5.6. Characterization of Pt@UiO-66-NH2 Thin Film on substrates 80 5.6.1. Thin Film Growth on α-Al2O3 substrate 80 5.6.2. Thin Film Growth on FTO 87 6. Conclusion 93 7. Future Prospects 94 8. Reference 95 Appendix 102 A.1 ICP calibration curve of zirconium and platinum 102 A.2 Characterization of α-Al2O3 substrate 103 A.3 Characterization of FTO substrate 104 A.4 XRD Pattern of Simulated UiO-66-NH2 and Pt 105 | |
| dc.language.iso | en | |
| dc.title | 以原位合成法(De Novo Synthesis)製備胺官能化UiO-66金屬有機骨架孔洞材料搭載鉑奈米粒子之粉粒及薄膜 | zh_TW |
| dc.title | De Novo Synthesis of Pt-embedded Metal-Organic Frameworks (UiO-66-NH2) Particles and Films | en |
| dc.type | Thesis | |
| dc.date.schoolyear | 106-2 | |
| dc.description.degree | 碩士 | |
| dc.contributor.oralexamcommittee | 謝發坤(Fa-Kuen Shieh),林嘉和(Chia-Her Lin),童國倫(Kuo-Lun Tung),蔡德豪(De-Hao Tsai) | |
| dc.subject.keyword | 金屬有機骨架,原位合成法,金屬有機骨架衍生異相觸媒,UiO-66,金屬有機骨架薄膜, | zh_TW |
| dc.subject.keyword | Metal-organic frameworks,de novo synthesis,MOF-derived heterogeneous catalysts,UiO-66,MOF thin film, | en |
| dc.relation.page | 105 | |
| dc.identifier.doi | 10.6342/NTU201801062 | |
| dc.rights.note | 有償授權 | |
| dc.date.accepted | 2018-06-25 | |
| 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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