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研究生：	石家聲 Shih, Chia-Sheng
論文名稱：	以Mn2O3/Al2SiO5固定床反應器探討低溫下觸媒氧化苯乙烯之研究 Catalytic Oxidation of Styrene by Mn2O3/Al2SiO5 at Low Temperature in a Fixed Bed Reactor
指導教授：	朱信 Chu, Hsin
學位類別：	碩士 Master
系所名稱：	工學院 - 環境工程學系 Department of Environmental Engineering
論文出版年：	2021
畢業學年度：	109
語文別：	英文
論文頁數：	143
中文關鍵詞：	觸媒氧化、錳觸媒、固定床反應器、降解苯乙烯
外文關鍵詞：	Catalytic oxidation, Mn-based catalyst, Fixed bed reactor, Styrene
相關次數：	點閱：102 下載：0
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近年來隨著人口的增加以及自工業革命以來科技的快速發展，對於能源的需求不斷增加。而能源的主要來源為化石燃料，化石燃料帶來的問題不僅有二氧化碳的排放，還有揮發性有機物(VOCs)的問題。苯乙烯廣泛應用於石化業，包括塑膠、橡膠合成等。觸媒氧化技術是目前被視為有潛力且具經濟效益之技術。本研究使用臨濕含浸法自製一系列不同比例的Mn2O3/Al2SiO5為觸媒並在標準條件下（100 ppm苯乙烯、10,000 hr-1和21% O2）與苯乙烯反應，以尋找最佳比例-38wt% Mn2O3/Al2SiO5。在TGA分析中，Mn(NO3)2．4H2O/Al2SiO5在600oC通以空氣鍛燒下重量下降至原先的31.1%。根據重量損失，觸媒還原為Mn2O3狀態。選定38wt% Mn2O3/Al2SiO5觸媒後，進行參數實驗探討不同操作條件(氣體濃度、氣體流速、溫度)對觸媒反應性的影響。在固定床反應器實驗中，轉化率會隨著苯乙烯濃度的增加而降低，因為觸媒的活性位點被占據而飽和。當空間流速變低時，相同溫度下的轉化率越來越高。在氧濃度的參數中，除氧濃度為0%的條件之外，其他氧濃度條件下的轉化率幾乎相同。值得注意的是，0%氧濃度條件下的催化劑由Mn2O3還原為Mn3O4。觸媒失活實驗中，在165oC下進行 3 天反應後，觀察到了積碳，38wt% Mn2O3/Al2SiO5對苯乙烯的轉化率下降到30%。從XRD、XPS、FTIR和SEM的結果顯示，除了參數實驗中0%氧的情況下38wt% Mn2O3/Al2SiO5中的Mn2O3被還原為Mn3O4之外，其餘結果均顯示觸媒在200oC具有優異的耐受性，並且在較高的溫度下可延緩苯乙烯引起的積碳。

In recent years, with the expanding of population and the development of industry revolution, the energy demand continuously increases. The main source of energy comes from the combustion of fossil fuel, and it causes big problems, not only the problem of carbon dioxide generation, but also volatile organic compounds (VOCs). Styrene is widely used in the petrochemical industry, including plastics, rubber synthesis, medical synthesis and nitrocellulose plastics, etc. Catalytic oxidation technology is one of the promising technologies for the abatement of exhaust gases. In this study, a series of Mn2O3/Al2SiO5 catalysts in different proportions, prepared by the incipient wetness impregnation method, were used to react styrene under standard condition (100 ppm styrene, 10,000 hr-1 and 21% O2) to find the best ratio, 38wt% Mn2O3/Al2SiO5. In TGA experiment, the weight of Mn(NO3)2．4H2O/Al2SiO5 is reduced to 31.1% by air in 600oC. According to the weight loss, the catalyst is reduced to the state Mn2O3. The 38wt% Mn2O3/Al2SiO5 catalyst was used to react with simulated styrene exhaust gas under various reaction conditions to investigate the reactivity of catalysts under various operation conditions. In parameter experiments, results show that conversion of catalysts would decrease with increasing styrene concentration due to their active sites saturation. When space velocity becomes lower, the conversions at the same temperature are getting higher and reach saturation at lower temperature. Except in the condition of 0% oxygen concentration, the conversions under other oxygen concentration conditions are almost the same, with only little differences. It is worth noting that the catalyst in the condition of 0% oxygen concentration is reduced from Mn2O3 to Mn3O4. There is a carbon masking problem from the catalytic deactivation test. After 3 days experiment at 165oC, the conversion of styrene by 38wt% Mn2O3/Al2SiO5 decreases to about 30% due to the formation of carbon deposits. From the results of XRD, XPS, FTIR and SEM, except in the case of 0% oxygen in the parameter experiment, Mn2O3 in 38wt% Mn2O3/Al2SiO5 is reduced to Mn3O4, the rest of the results all show the rest show that the catalyst has excellent durability when the operating temperature increases from 165 to 200oC. It can retard the carbon deposit caused by styrene at higher temperature.

摘要 I
Abstract II
誌謝 IV
Content VI
List of tables X
List of figures XII
Chapter 1 Introduction 1
1-1 Motivation 1
1-2 Objectives 3
Chapter 2 Literature and Review	4
2-1 Introduction of VOCs 4
2-1.1 Definition of VOCs 4
2-1.2 The main source of VOCs 8
2-1.3 Influence of VOCs 10
2-2 Characteristics of styrene 12
2-2.1 Property of styrene 12
2-2.2 Sources and use of styrene 15
2-2.3 Hazards of styrene 15
2-3 Control method of VOCs 18
2-4 Catalytic oxidation	20
2-4.1 Characteristics of catalytic oxidation 20
2-4.2 Mechanisms for catalytic oxidation 21
2-4.3 Calculation of catalyst oxidation efficiency 23
2-4.4 Impact factors of catalytic oxidation activity 25
2-5 Characteristics of catalyst	27
2-5.1 Mn-based catalyst	27
2-5.2 Ni-based catalyst	28
2-5.3 Cu-based catalyst	28
2-5.4 Fe-based catalyst	29
2-6 Preparation of catalyst 30
2-6.1 Mechanical mixing 30
2-6.2 Co-precipitation 30
2-6.3 Sol-gel 31
2-6.4 Incipient wetness impregnation 31
2-6.5 Freeze granulation 31
2-7 Deactivation of catalyst 33
2-7.1 Fouling 33
2-7.2 Sintering 33
2-7.3 Losses of active sites 34
2-7.4 Poisoning	34
2-8 Catalytic oxidation reaction kinetics 35
2-8.1 Plug flow reactor	37
2-8.2 Catalytic kinetics model 40
2-8.3 Arrhenius equation 46
Chapter 3 Material and methods 47
3-1 Experimental methods 47
3-1.1 Experimental design 48
3-1.2 Experimental process 50
3-2 Experimental equipment 52
3-2.1 Experimental materials 52
3-2.2 Experimental facilities 53
3-2.3 Analyzer 59
3-3 Preliminary experiment 67
3-3.1 Preparation of catalyst 67
3-3.2 Calibration curve preparation 69
3-3.3 Leakage proof of the system 71
3-3.4 Stability test of the exhaust gas simulation system 71
Chapter 4 Results and Discussion 73
4-1 Characteristic of catalysts 73
4-1.1 Thermogravimetric Analysis (TGA) 73
4-1.2 Catalytic effect 76
4-1.3 BET surface area analysis 79
4-1.4 X-ray diffraction (XRD) analysis 85
4-1.5 Inductively couple plasma optical emission spectrometry (ICP-OES) 86
4-2 Operating parameters experiment 87
4-2.1 Styrene concentration 89
4-2.2 Space velocity 91
4-2.3 Oxygen concentration 93
4-2.4 Catalytic deactivation test 95
4-3 Characteristic of catalysts before and after the reaction 97
4-3.1 X-ray diffraction (XRD) analysis 97
4-3.2 Scanning electron microscope (SEM) analysis 100
4-3.3 Scanning electron microscope with energy dispersive spectroscopy (SEM-EDS) analysis 103
4-3.4 Mapping analysis 106
4-3.5 X-ray photoelectron spectroscope (XPS) analysis 109
4-3.6 Fourier transform infrared (FTIR) analysis 113
4-4 Kinetics 114
4-4.1 power-rate law 114
4-4.2 Mars＆Van-Krevelen (MVK) model 120
4-4.3 Langmiur-Hinshelwood model 123
4-5 Mechanisms 130
4-5.1 Mineralization of analysis 130
Chapter 5 Conclusion and suggestion 131
5-1 Conclusion 131
5-2 Suggestion 133
Chapter 6 Reference 134
                                    

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