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http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/22477完整後設資料紀錄
| DC 欄位 | 值 | 語言 |
|---|---|---|
| dc.contributor.advisor | Jeffrey Chi-Sheng Wu(吳紀聖) | |
| dc.contributor.author | Van-Huy Nguyen | en |
| dc.contributor.author | 胡阮凡 | zh_TW |
| dc.date.accessioned | 2021-06-08T04:18:42Z | - |
| dc.date.copyright | 2010-07-29 | |
| dc.date.issued | 2010 | |
| dc.date.submitted | 2010-07-26 | |
| dc.identifier.citation | [1] ICIS Chemical Business (ICB) Chemical Profile (September 2007 ed.). (2007), Available: http://www.icis.com
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| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/22477 | - |
| dc.description.abstract | 近年來有許多學者致力於環氧化反應的研究，然而在大多的反應情形中，都伴隨著廢水廢熱問題，且產物需要經由分離再純化，經濟效益也不高，且最大的問題在於反應形成環氧丙烷的轉化率和選擇率都仍然很低。從經濟效益和環境保護的觀點來看，氧氣是相當理想的氧化劑，可用來跟丙烯選擇性反應生成環氧丙烷，已經有一些研究致力於發展這樣的乾淨製程，藉由提供光能給光觸媒材料，便可輔助氣相原料間的直接氧化反應產生環氧丙烷，這是相當具有前景的化學品生產途徑。
本研究目標在研究不同種類的光觸媒於室溫下進行光催化環氧反應，希望能提升目標產物環氧丙烷(PO)的選擇率。負載金的TiO2和釩的SiO2光觸媒是分別由光沉積法和含浸法製得，TS-1則是經由水熱結晶法製備。在多組實驗結果中，最佳反應條件為使用TS-1觸媒，在50oC一大氣壓下照射強度1W/cm2 之UVA紫外光，進料流速3000ml/h，反應四小時可得PO產率28.75μmol.g-cat−1.h−1，且PO選擇率達43.2%。此外，在相同條件下若使用Au(0.1 wt%)/TS-1觸媒，可進一步觀察到反應生成PO的平均產率能維持在24-26 μmol.g-cat–1.h–1達15小時，失活情形大為減少。 | zh_TW |
| dc.description.abstract | In recent years, there has been great research focus on epoxidation; however, in most case, we face the disposal, separation, and economic problems. In addition, the propylene conversion and the selectivity to propylene oxide (PO) are still very low. Molecular oxygen is an ideal oxidant for a selective epoxidation of propylene from the environmental and economic viewpoints. A major research effort has been made in the development of alternative direct epoxidation processes for the production of propylene oxide. The aim is to develop a process for the direct gas-phase photo epoxidation. With the aid of light energy and heterogeneous photocatalyst, it is promising for chemicals production. Therefore, this research explores the photo selective catalytic epoxidation of propylene via O2.
The key is using photo-energy to achieve higher epoxidation products selectivity at room temperature over series of photocatalysts. The catalysts used in this research are the supported gold on TiO2, vanadium loaded SiO2 and titanium silicalite (TS-1) prepared by photo-deposition method, impregnation method and hydrothermal crystallization of gel, respectively. The most favorable photocatalytic epoxidation, with 28.75μmol.g-cat−1.h−1 highest PO specific rate and 43.2% PO selectivity obtained on stream after 4 hrs, was TS-1 photocatalysts under the 3,000 ml.h−1, 1W/cm2 UVA irradiation and very mild conditions (50oC and atmospheric pressure). In addition, the epoxidation was conducted over Au(0.1 wt%)/TS-1 with significant improvement on the lifetime and still achieved ~ 24-26 μmol.g-cat–1.h–1 PO specific rate on stream after 15 hrs. | en |
| dc.description.provenance | Made available in DSpace on 2021-06-08T04:18:42Z (GMT). No. of bitstreams: 1 ntu-99-R97524092-1.pdf: 12407526 bytes, checksum: 4a08699a5e4ac1be45bb862b77be9d27 (MD5) Previous issue date: 2010 | en |
| dc.description.tableofcontents | Abstract I
Abstract (Chinese) II Contents III List of Figures VI List of Tables XIII 1 Introduction 1 1.1 Background 1 1.2 Research Motivations 3 1.3 Research Goals 3 2 Literature Survey 4 2.1 Background of Photocatalysis 4 2.1.1 Introduction to TiO2 5 2.1.2 Semiconductor under Excitation 8 2.2 Epoxides Background 10 2.2.1 Epoxides Reactions 11 2.2.2 The Catalytic Mechanisms of Epoxidation 13 2.2.3 Industrially Important Epoxides 15 2.3 Background of Propylene Oxide 19 2.3.1 Introduction 19 2.3.2 Chemical Properties 19 2.3.3 Physical Properties 21 2.3.4 Uses for Propylene Oxide 22 2.3.5 Aspects 23 2.4 Production and Raw Materials from Manufacture of Propylene Oxide 24 2.4.1 Production Route via Propylene Chlorohydrin (CHPO) 27 2.4.2 Production Route via Propylene Co-products 35 2.4.3 Production Route via Hydrogen Peroxide (HPPO) 44 2.4.4 Production Route via Direct Oxidation 46 2.4.5 Production Route via Electrochemical Process 46 2.4.6 Production Route via Biochemical Processes 47 2.5 Selective Catalytic Epoxidation 48 2.5.1 Motivate of Selective Catalytic Epoxidation 48 2.5.2 Directly Photo Selective Catalytic is the Future for Epoxidation 57 3 Experimental 58 3.1 Materials and Apparatus 58 3.1.1 Chemicals 58 3.1.2 Apparatus 59 3.2 Preparation of Photocatalysts 61 3.2.1 Amorphous SiO2 61 3.2.2 V2O5(0.5 wt%)/SiO2 62 3.2.3 Au(x wt%)/TiO2 63 3.2.4 Titanium silicalite (TS-1) 64 3.2.5 Au (0.1 wt%)/TS-1 66 3.3 Photocatalyst Characterization 66 3.3.1 X-Ray Diffraction (XRD) 66 3.3.2 UV-Visible Spectrometer 70 3.3.3 Field Emission Scanning Electron Microscopy (SEM) 71 3.3.4 Energy Dispersive Spectrometer (EDS) 72 3.3.5 Surface Area Measurement by N2 adsorption 73 3.3.6 X-ray Photoelectron Spectroscopy (XPS) 74 3.3.7 Gas Chromatograph Instrument 74 3.4 Photo Selective Catalytic Epoxidation System 84 3.4.1 Reaction System 84 3.4.2 Photo-reactor 86 3.4.3 Light sources 89 4 Results and Discussion 91 4.1 Catalyst Characterization 91 4.1.1 UV-Visible Spectroscopy 91 4.1.2 XRD 93 4.1.3 BET 98 4.1.4 SEM 99 4.1.5 TEM 103 4.1.6 EDS 106 4.1.7 XPS 107 4.2 Photocatalytic epoxide reaction 113 4.2.1 Blank experiments 113 4.2.2 C3H6 Adsorption 114 4.2.3 Photocatalytic epoxidation over TS-1 117 4.2.4 Photocatalytic epoxidation over Au(0.1wt%)/TS-1 124 4.2.5 Photocatalytic epoxidation over P25 127 4.2.6 Photocatalytic epoxidation over Au(0.5 wt%)/TiO2 non calcined 129 4.2.7 Photocatalytic epoxidation over Au(0.5 wt%)/TiO2 130 4.2.8 Photocatalytic epoxidation over Au(3 wt%)/TiO2 132 4.2.9 Photocatalytic epoxidation over Au(2-3 wt%)/TiO2 132 4.2.10 Photocatalytic epoxidation over SiO2_synthesis 134 4.2.11 Photocatalytic epoxidation over V2O5(0.5 wt%)/SiO2 commercial 135 4.2.12 Effect of the light intensity on photocatalytic epoxidation 136 4.2.13 Effect of the temperature on photocatalytic epoxidation 140 5 Summary 142 5.1 Reaction Mechanism of Photo-epoxidation by Propylene 142 5.2 The Role of the Silica Supports 145 5.3 The Carbon Loss 146 5.4 Propylene Oxide Production 147 5.5 Comparison the Epoxidation Results from The Others Group 148 6 Conclusions 151 References 152 Appendices 163 Author's Biography 166 | |
| dc.language.iso | en | |
| dc.subject | 環氧化 | zh_TW |
| dc.subject | 氧氣. | zh_TW |
| dc.subject | 環氧丙烷 | zh_TW |
| dc.subject | 光觸媒 | zh_TW |
| dc.subject | Epoxidation | en |
| dc.subject | photocatalyst | en |
| dc.subject | oxygen. | en |
| dc.subject | propylene oxide | en |
| dc.title | 光催化環氧化丙烯之研究 | zh_TW |
| dc.title | Photocatalytic Epoxidation of Propylene with Molecular Oxygen | en |
| dc.type | Thesis | |
| dc.date.schoolyear | 98-2 | |
| dc.description.degree | 碩士 | |
| dc.contributor.oralexamcommittee | 萬本儒(Ben-Zu Wan),白曛綾(Hsun-Ling Bai) | |
| dc.subject.keyword | 環氧化,環氧丙烷,光觸媒,氧氣., | zh_TW |
| dc.subject.keyword | Epoxidation,propylene oxide,photocatalyst,oxygen., | en |
| dc.relation.page | 166 | |
| dc.rights.note | 未授權 | |
| dc.date.accepted | 2010-07-27 | |
| 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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