臺灣博碩士論文加值系統

化學迴路部分氧化程序相較傳統的氣化程序顯示出一些優勢，不但能避免燃料的過度氧化成二氧化碳與蒸氣，並能產出高質量的合成氣當作化學品工業的原料物。本研究主要目的在於製備出二鈣鐵載氧體，並運用於同向流移動床反應器中分別與甲烷和RDF 進行化學迴路部分氧化之評估。
二鈣鐵載氧體的組成鈣鐵莫爾比為50：50，且於1150℃下進行鍛燒，此載氧體展現出優異的合成氣選擇性、循環再生性、破碎強度，並具有較低的磨耗。DCaF-1150載氧體的還原機制在合成氣氛下進行檢測，實驗結果顯示：二鈣鐵載氧體會直接被還原成氧化鈣與金屬鐵，不需經過氧化鐵相態，且無其他鈣鐵相態生成。此外DCaF-1150載氧體的還原動力式也分別於氫氣與一氧化碳氣氛下進行測試，氫氣氣氛下的還原活化能為84.30 kJ/mol，另一方面，一氧化碳氣氛下的還原活化能為69.22 kJ/mol。
於最佳操作參數下，甲烷部分氧化使用蒸氣當作氣化劑的實驗顯示碳轉化率約為81.42%，合成氣濃度約為86.39 mol.%。甲烷部分氧化使用二氧化碳當作氣化劑的實驗顯示碳轉化率約為81.63%，合成氣濃度約為84.20 mol.%。
於最佳操作參數下，RDF部分氧化使用蒸氣當作氣化劑的實驗顯示碳轉化率約為59.56%，合成氣濃度約為85.84 mol.%。RDF部分氧化使用二氧化碳當作氣化劑的實驗顯示碳轉化率約為68.20%，合成氣濃度約為82.11 mol.%。
本研究成功製備出二鈣鐵載氧體，並運用於同向流移動床反應器中進行化學迴路部分氧化，研究結果指出鈣鐵系列當作載氧體具有較佳的潛力運用於合成氣的產出，可以符合不同化學工業製程上之需求。

Chemical looping partial oxidation process demonstrates better advantages than conventional gasification process, which can not only avoid completely oxidizing fuel into CO2 and H2O, but also supply high quality of syngas for feedstock of chemicals industrial. In this study, di-calcium ferrite oxygen carriers are developed to conduct the investigation on chemical looping partial oxidation of methane and RDF.
Di-calcium ferrite (DCaF) oxygen carriers are prepared with iron/calcium mole ratio of 50/50. The oxygen carriers calcined at 1150℃ exhibits good syngas selectivity, recyclability, crush strength and lower attrition. The reduction mechanism of DCaF-1150 is carried out under syngas atmosphere, the results indicate that Ca2Fe2O5 is directly reduced into metallic iron and CaO, without passing through any iron oxides and no other crystalline phase of calcium ferrite formed. The reduction kinetics analysis is individually discussed under hydrogen or carbon monoxide atmosphere, the apparent activation energy of reduction under H2 atmosphere was 84.30 kJ/mol; on the other hand, the apparent activation energy of reduction under CO atmosphere was 69.22 kJ/mol.
Under optimal operation condition, the experiment of methane partial oxidation using steam as gasification agent shows the carbon conversion is approximately 81.42%, syngas concentration is approximately 86.39 mol.%. The experiment of methane partial oxidation using CO2 as gasification agent shows the carbon conversion is approximately 81.63%, syngas concentration is approximately 84.20 mol.%.
Under optimal operation condition, the experiment of RDF partial oxidation using steam as gasification agent shows the carbon conversion is approximately 59.56%, syngas concentration is approximately 85.84 mol.%. The experiment of RDF partial oxidation using CO2 as gasification agent shows the carbon conversion is approximately 68.20%, syngas concentration is approximately 82.11 mol.%.
The di-calcium ferrite oxygen carriers are successful prepared for chemical looping partial oxidation in a co-current moving bed reactor. The results indicate that calcium ferrite oxygen carriers demonstrate potential applications on syngas production for different processes of chemical industrial.

中文摘要 I
Abstract III
Acknowledgement V
Table of Contents VII
List of Figures XI
List of Tables XV
List of Symbols XVII
Chapter 1 Introduction 1
1.1 Background 1
1.2 Objective and Scope 3
Chapter 2 Literature and Review 5
2.1 Chemical Looping Processes 5
2.1.1 Chemical Looping Combustion 5
2.1.2 Chemical Looping Partial Oxidation 11
2.1.3 Biomass Applications by using Chemical Looping Processes 15
2.2 Oxygen Carriers for Chemical Looping Processes 21
2.2.1 Development of the Iron-Based Oxygen Carriers 23
2.2.2 Development of the Calcium Ferrite Oxygen Carriers 26
2.2.3 Reaction Kinetics Analysis of the Oxygen Carriers 30
2.3 Syngas Generation by using Chemical Looping Processes 35
2.3.1 Conventional Syngas Generation from Fuel Gasification and Reforming 36
2.3.2 Syngas Generation by Moving Bed Reactor 39
2.3.3 High Quality Syngas Production from Chemical Looping Processes 43
2.4 Optimal Operating Parameters for Chemical Looping Processes 45
2.4.1 Effect of Fuel Reactor Temperature 45
2.4.2 Effect of Oxygen Carriers to Solid Fuel Ratio 47
2.4.3 Effect of Gasification Agent Flow Rate 48
Chapter 3 Experimental Apparatus and Procedures 51
3.1 Materials 51
3.2 Apparatus and Instruments 52
3.3 Experimental Procedures 53
3.3.1 Experiment Framework 53
3.3.2 Preparation of Di-Calcium Ferrite Oxygen Carriers 62
3.3.3 System of Chemical Looping Process 63
3.3.4 Characterization Analysis of Di-Calcium Ferrite Oxygen Carriers 72
3.3.5 Method of Analysis RDF and Data Evaluation 75
Chapter 4 Results and Discussion 79
4.1 Oxygen Carriers Preparation 80
4.1.1 Reactivity and Recyclability of Di-Calcium Ferrite Oxygen Carriers 80
4.1.2 Characterization of Di-Calcium Ferrite Oxygen Carriers 84
4.1.3 Crush Strength and Attrition of Di-Calcium Ferrite Oxygen Carriers 88
4.1.4 Reduction Mechanism of Di-Calcium Ferrite Oxygen Carriers 90
4.1.5 Reduction Kinetics Analysis of Di-Calcium Ferrite Oxygen Carriers under Different Fuel Gas Atmosphere 93
4.2 Methane Partial Oxidation with Di-Calcium Ferrite Oxygen Carriers in a Co-Current Moving Bed Reactor 103
4.2.1 Methane Reforming in an Empty Moving Bed Reactor 103
4.2.2 Effect of Fuel Reactor Temperature on Methane Partial Oxidation 108
4.2.3 Effect of Oxygen to CH4 Ratio on Methane Partial Oxidation 115
4.2.4 Effect of Gasification Agent to CH4 Ratio on Methane Partial Oxidation 122
4.3 Refuse-Derived Fuel (RDF) Partial Oxidation with Di-Calcium Ferrite Oxygen Carriers in a Co-Current Moving Bed Reactor 128
4.3.1 RDF Gasification in an Empty Moving Bed Reactor 128
4.3.2 Effect of Fuel Reactor Temperature on RDF Partial Oxidation 132
4.3.3 Effect of Oxygen Carriers to Carbon Ratio on RDF Partial Oxidation 139
4.3.4 Effect of Gasification Agent to Carbon Ratio on RDF Partial Oxidation 145
Chapter 5 Conclusions and Recommendations 151
References 157
Appendix 167
Curriculum Vitae 169

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