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完整後設資料紀錄
DC 欄位 | 值 | 語言 |
---|---|---|
dc.contributor.advisor | 吳嘉文(Chia-Wen Wu) | |
dc.contributor.author | Yen-Tsz Bieh | en |
dc.contributor.author | 畢晏慈 | zh_TW |
dc.date.accessioned | 2021-07-11T14:52:53Z | - |
dc.date.available | 2022-07-31 | |
dc.date.copyright | 2020-08-04 | |
dc.date.issued | 2020 | |
dc.date.submitted | 2020-07-27 | |
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dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/78358 | - |
dc.description.abstract | 聚對苯二甲酸乙二酯是一種熱塑性聚酯,因為已被廣泛用於製造各種包裝,因此導致有將近數百萬噸的聚對苯二甲酸乙二酯廢棄物被產生出來。隨著聚對苯二甲酸乙二酯廢塑料數量的增加,如何將其有效地回收或降解已被認定為一項需要解決的重要議題。目前有很多種降解聚對苯二甲酸乙二酯的方法,在眾多降解廢塑料的方法之中,糖解是一種具有較多優勢的解聚方式,除了反應可在相對較溫和的條件下進行以外,聚對苯二甲酸乙二酯廢棄物的糖解可產生對苯二甲酸雙(2-羥乙基)酯(BHET)單體,其可作為重新合成聚對苯二甲酸乙二酯過程中的原料。 本團隊開發出一套藉由糖解反應來回收廢塑料(聚對苯二甲酸乙二酯)的系統,並使用含鋅金屬多氮唑框架(MAF-6)觸媒來催化,於乙二醇環境下解聚聚對苯二甲酸乙二酯,生產BHET單體。MAF-6是金屬有機框架(MOF)的子類,由金屬離子(Zn2+)和有機配位體(2-乙基咪唑)所組成。本研究仔細地探討了一系列的反應參數對PET糖解性能的影響,其中包括反應溫度、反應時間和催化劑用量。使用MAF-6觸媒,在180°C和4 h的反應條件下,聚對苯二甲酸乙二酯的轉化率高達92.4 %,BHET單體的產率為81.7%。因為MAF-6為非均相觸媒,因此有易於回收之特性,而且可以重複使用至少五次以上,PET的轉化率(91.0 %)和BHET單體的產率(71.2 %)也都能維持在一定的水準之上。此外,可能的反應機制也被提出,由動力學分析得知,聚對苯二甲酸乙二酯的糖解反應過程為一級反應,其活化能為197.3 kJ / mol。基於這些實驗結果,本團隊所提出聚對苯二甲酸乙二酯廢塑料降解之系統在永續社會中具有實際應用的潛力。 | zh_TW |
dc.description.abstract | Polyethylene terephthalate (PET) is a thermoplastic polyester which has been extensively used as fabrication of various kinds of packaging, creating millions of tons of PET wastes. With the increase of PET wastes, recycling or degrading PET wastes has been identified as a prominent issue which needs to be solved. One of the promising degradation process for PET is glycolysis which could be conducted under mild reaction conditions comparing with other methods. Furthermore, glycolysis of PET wastes can generate bis(2-hydroxyethylterephthalate) (BHET) monomeric product as the raw material in the synthesis of PET. Herein, an effective catalytic process for the chemical recycling of PET has been demonstrated by using Metal Azolate Framework-6 (MAF-6) catalyst in the presence of ethylene glycol to generate bis(2-hydroxyethylterephthalate) (BHET) monomeric product. MAF-6, a subclass of metal-organic frameworks (MOFs), is comprised of metal ion (Zn2+) and organic ligand (2-ethylimidazole). The effects of reaction parameters including reaction temperature, reaction time, and the amount of catalyst on PET glycolysis performance were scrutinized. Up to 92.4% conversion of PET and 81.7% yield of BHET were achieved over MAF-6 catalyst under reaction condition of 180 °C and 4 h. MAF-6 catalyst can be easily recovered and reused for at least five times, and the conversion of PET and yield of BHET remained stable at 91.0% and 71.2%, respectively. Additionally, a possible mechanism of PET glycolysis reaction catalyzed by MAF-6 was proposed. Furthermore, PET glycolysis process is considered as the pseudo first-order reaction and the activation energy is 197.3 kJ/mol. Based on these experimental results, this work has great potential in PET wastes degradation and can be possible for further industrial application. | en |
dc.description.provenance | Made available in DSpace on 2021-07-11T14:52:53Z (GMT). No. of bitstreams: 1 U0001-2407202014282000.pdf: 6129785 bytes, checksum: 69f98ebc15a189e43ec04d0aaed8e96d (MD5) Previous issue date: 2020 | en |
dc.description.tableofcontents | ABSTRACT i 摘要 ii Table of Content iii List of Figures v List of Tables vii 1. Introduction 1 1.1. Polyethylene terephthalate (PET) 1 1.2. Bis(2-Hydroxyethyl) terephthalate (BHET) 2 1.3. Global plastic production 3 1.4. Recycling process of plastic waste 4 1.4.1. Primary recycling 4 1.4.2. Physical recycling 5 1.4.3. Energy recovery (Incineration) 5 1.4.4. Chemical recycling 6 1.5. Glycolytic chemical recycling of PET 7 1.6. Selection of catalyst 8 1.6.1. Metal Organic Framework (MOFs) 8 1.6.2. Metal Azolate Framework (MAFs) 9 2. Literature Review 13 3. Objective 17 4. Experimental 18 4.1. Chemicals and materials 18 4.2. Equipment 19 4.3. Preparation of catalysts 21 4.4. Glycolysis reaction of PET 22 4.5. Characterizations of monomeric product (BHET) 24 4.5.1. Calculation Formula of PET Conversion and BHET Yield 24 4.5.2. Gas Chromatograph-Flame Ionization Detector (GC-FID) 24 4.5.3. Gas Chromatography-Mass Spectrometer (GC-MS) 25 4.5.4. Differential Scanning Calorimetry/Thermogravimetry (DSC/TGA) 25 4.5.5. Elemental Analyzer (EA) 26 4.5.6. Nuclear Magnetic Resonance Spectroscopy (NMR) 26 4.5.7. Fourier-Transform Infrared Spectroscopy (FTIR) 26 4.6. Characterizations of catalysts 27 4.6.1. Powder X-ray diffractometer (PXRD) 27 4.6.2. Field Emission Scanning Electron Microscope (FE-SEM) 27 4.6.3. Specific Surface Area Pore Size Distribution Analyzer 28 4.6.4. Differential Scanning Calorimetry/Thermogravimetry (DSC/TGA) 28 4.6.5. Inductively Coupled Plasma-Mass Spectrometer (ICP-MS) 29 5. Results and Discussions 30 5.1. Characterizations of catalysts 30 5.1.1. PXRD analysis 30 5.1.2. SEM analysis 31 5.1.3. N2 physisorption analysis 32 5.1.4. IR analysis of pyridine adsorption 33 5.2. Reaction optimization of MAF-6 34 5.2.1. The effect of amount of catalyst 35 5.2.2. The effect of reaction temperature 36 5.2.3. The effect of reaction time 37 5.2.4. Evaluation test of commercial and MAF catalysts 38 5.2.5. Summary in optimizing condition 39 5.3. Characterizations of monomeric product (BHET) 40 5.4. Reusability test 43 5.5. Affinity evaluations 44 5.6. Reaction mechanism studies 50 5.7. Practical application 53 5.8. Kinetic evaluations 55 6. Conclusion 58 7. Future Prospect 59 Reference 60 Appendix 66 | |
dc.language.iso | en | |
dc.title | 高密度鋅之金屬有機框架(MAF-6)應用於聚對苯二甲酸乙二酯(PET)的轉化反應 | zh_TW |
dc.title | Heterogeneous Metal Azolate Framework-6 (MAF-6) Catalyst with High Zinc Density for Enhanced Polyethylene terephthalate (PET) Conversion | en |
dc.type | Thesis | |
dc.date.schoolyear | 108-2 | |
dc.description.degree | 碩士 | |
dc.contributor.oralexamcommittee | 謝發坤(Fa-Kuen Shieh),張嘉修(Jo-Shu Chang),蘇銘千(Ming-Chien Su),黃郁慈(Yu-Tzu Huang) | |
dc.subject.keyword | 聚對苯二甲酸乙二酯,金屬多氮唑框架材料,糖解反應,廢棄物回收處理,高分子解聚, | zh_TW |
dc.subject.keyword | Polyethylene terephthalate (PET),Metal azolate frameworks (MAFs),Glycolysis reaction,Waste recycling treatment,Polymer depolymerization, | en |
dc.relation.page | 69 | |
dc.identifier.doi | 10.6342/NTU202001824 | |
dc.rights.note | 有償授權 | |
dc.date.accepted | 2020-07-28 | |
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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