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研究生: 黃冠傑
Huang, Kuan-Chieh
論文名稱: 利用田口法研究汙水污泥和廢塑料之共熱解特性
A Study of Co-pyrolysis Characteristics of Sewage Sludge and Waste Plastics Using Taguchi Method
指導教授: 陳冠邦
Chen, Guan-Bang
學位類別: 碩士
Master
系所名稱: 工學院 - 航空太空工程學系
Department of Aeronautics & Astronautics
論文出版年: 2022
畢業學年度: 110
語文別: 英文
論文頁數: 104
中文關鍵詞: 汙水汙泥廢塑料廢聚丙烯共熱解催化熱解田口實驗法
外文關鍵詞: Sewage sludge, Waste plastics, Waste polypropylene, Co-pyrolysis, Catalytic pyrolysis, Taguchi’s experimental method
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  • 汙水汙泥和廢塑料近年來迅速累積,而傳統以掩埋處理的方式已面臨困境,所造成的環境問題若再繼續惡化,我們的生存環境最終將會難以挽回。而熱裂解提供了可有效去化廢棄物解決方法,能生成多種有價值的產物,並可透過調整實驗操作參數來改變所需產物(液態油、固態或液體)產率和品質。汙水汙泥(SS)具有低熱值、高灰分等特性,廢聚丙烯(PP)則是具有高熱值,高揮發分等特性;本研究藉由共熱解的方式,同時改善汙泥熱解油的品質和塑料本身特性所導致的實驗操作問題。本研究分析SS與PP的性質,利用TG-FTIR實驗探討其共熱解特性、並分析活化能變化、協同效應和產氣分析等。本研究利用田口法來找出製程最適化的三個目標(最佳產油率、最佳碳數比、最佳品質)。最佳產油率實驗操作參數為:原料為純SS、熱解溫度為500°C、料源滯留時間為1 hr、N2流率為200 mL/min,最佳產油率為13.33%;最佳碳數比(C5-12/C19+)實驗操作參數為:原料混合比為PP:SS=3:7、熱解溫度為450°C、料源滯留時間為1 hr、N2流率為400 mL/min,最佳C5-12/C19+為9.1;最佳熱解油品質實驗操作參數為: 原料混合比為PP:SS=1:9、熱解溫度為450°C、料源滯留時間為1.5 hr、N2流率為600 mL/min,石化產物成分(烯類+單芳香)與無價值產物(多環芳香+環狀化合物)最佳比值為4.02。將三個目標的最佳實驗參數分別加入10%的HZSM-5和活性氧化鋁發現,HZSM-5在熱值、產油率(SS和PP的共熱解)、最佳碳數比、熱解油品質都有顯著提升;而活性氧化鋁則較不具備預期的結果,但在增加芳香族化合物產率上則具有明顯效果。

    Sewage sludge and waste plastics have accumulated rapidly in recent years, with traditional landfill treatment methods facing significant difficulties. The living environment also faces eventual irreparable damaged if such issues are not addressed. Pyrolysis, which can effectively decompose waste, may provide a solution to the abovementioned problems, as it can generate a variety of valuable products, with the yield and quality of the desired product (liquid oil, solid, or gas) controlled by adjusting the experimental operating conditions.
    Sewage sludge (SS) has a low heating value and a high ash content, while waste polypropylene (PP) has a high heating value and a high volatile content. Co-pyrolysis was used in this study to improve the quality of sewage sludge pyrolysis oil and address the experimental operating problems associated with the characteristics of the plastic itself. The properties of SS and PP were analyzed in this study, their co-pyrolysis characteristics discussed based on thermogravimetry combined with Fourier-transform infrared spectroscopy (TG-FTIR) experiments, changes in activation energy, synergistic effects, and the analysis of gas-production components. The Taguchi method was used to examine the three process optimization objectives (maximum oil yield, optimal carbon number ratio, and optimal quality). The operating conditions for achieving maximum oil yield were experimentally determined to include pure SS feedstock, a pyrolysis temperature of 500 °C, a feedstock residence time of 1 h , and a N2 flow rate of 200 mL/min, which led to an optimal oil yield of 13.33%. The operating conditions for achieving the optimal carbon number ratio (C5-12/C19+) were experimentally determined include a feedstock mixing ratio (PP:SS) of 3:7, a pyrolysis temperature of 450 °C, a feedstock residence time of 1 h , and a N2 flow rate of 400 mL/min, which led to an optimal C5-12/C19+ ratio of 9.1. The operating conditions for achieving optimal pyrolysis oil quality were experimentally determined include a feedstock mixing ratio (PP:SS) of 1:9, a pyrolysis temperature of 450 °C, a feedstock residence time of 1.5 h , and a N2 flow rate 600 mL/min, which gave an optimal petrochemical product component (alkenes + monoaromatics) to worthless product (polyaromatics + cyclic compounds) component ratio of 4.02. In addition, 10% H form Zeolite Socony Mobil–5 (HZSM-5) and activated alumina were also added as catalysts. HZSM-5 was found to significantly improve the heating value, oil yield (co-pyrolysis of SS and PP), carbon number ratio, and pyrolysis oil quality, whereas activated alumina did not deliver the desired results; rather, it clearly increased the aromatic compound yield.

    中文摘要 I ABSTRACT II ACKNOWLEDGEMENTS IV TABLE OF CONTENTS V LIST OF TABLES VIII LIST OF FIGURES XII CHAPTER1 INTRODUCTION 1 1.1 Research background 1 1.2 Sewage sludge 2 1.3 Waste plastics 4 1.4 Objectives and motivation 6 CHAPTER2 LITERATURE REVIEW AND STUDY PURPOSE 8 2.1 Co-pyrolysis of biomass and plastics 8 2.2 Catalytic co-pyrolysis 11 CHAPTER3 EXPERIMENTAL EQUIPMENT AND ANALYTICAL METHODS 14 3.1 Raw materials 14 3.2 Tubular furnace experimental equipment and procedures 17 3.3 Experimental analysis equipment 19 3.3.1 Calorimeter 19 3.3.2 Elemental analyzer (EA) 20 3.3.3 Proximate Analysis 21 3.3.4 Thermogravimetry combined with Fourier-transform infrared spectroscopy (TG-FTIR) 21 3.3.5 Gas chromatography–mass spectrometry (GC/MS) 24 3.4 The Taguchi experimental method 24 3.5 Reaction kinetics 28 3.6 Synergy 30 CHAPTER4 FUEL PROPERTY, THERMOGRAVIMETRIC, AND PYROLYSIS OIL COMPOSITION ANALYSES 32 4.1 Fuel properties of sewage sludge (SS) and polypropylene (PP) 32 4.2 TG-FTIR 34 4.2.1 Thermogravimetric analysis 34 4.2.2 FTIR analysis 38 4.2.3 Activation energy 41 4.2.4 Synergy 43 4.3 Taguchi’s experimental design 44 4.4 GC/MS 49 CHAPTER5 THE BEST CO-PYROLYSIS PROCESS AND COMPARISONS USING TWO DIFFERENT CATALYSTS 58 5.1 Using the Taguchi method to optimize the co-pyrolysis process 58 5.1.1 Operating conditions for achieving maximum co-pyrolysis oil yield 58 5.1.2 Operating conditions for achieving co-pyrolysis oil with the optimum carbon number ratio 64 5.1.3 Operating conditions for achieving optimum co-pyrolysis oil quality 69 5.2 Catalytic upgrading 77 5.2.1 Catalytic pyrolysis under optimal oil yield experimental conditions 78 5.2.2 Catalytic co-pyrolysis under optimal carbon number ratio conditions 80 5.2.3 Catalytic co-pyrolysis under optimum pyrolysis oil quality conditions 83 CHAPTER6 CONCLUSION 92 REFERENCES 96

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