臺灣博碩士論文加值系統

近年來經濟蓬勃發展，化石燃料已被人類廣泛使用，大量化石燃料燃燒釋放大量的二氧化碳加劇溫室效應影響。為了解決這些問題很多研究學家因此投入二氧化碳捕獲和封存技術研究。純氧燃燒系統是一種二氧化碳濃縮技術，在煙道尾氣端會排放高濃度的二氧化碳利於捕獲，並可以降低捕獲成本。因此本研究使用脫硫渣和水淬爐石作為固態吸附劑，不僅可降低吸附劑的成本，而且具有較高的鈣含量利於捕獲流化床反應器系統中煙道氣的二氧化碳和增加爐石再利用性。因此本研究模擬純氧燃燒之煙道氣條件，探討在流體化床反應系統中在高溫下使用脫硫渣和水淬爐石捕獲二氧化碳效果。
本研究操作條件及研究成果分為下列幾部分說明：
1.隨著溫度上升，在各種粒徑下的脫硫渣和水淬爐石的最小流化化速度經驗公式預測和實驗結果都是下降的趨勢。然而，爐渣顆粒的粒徑大小和比重也會影響各種溫度下最小流體化速度的數值。
2.根據TGA結果得知，脫硫渣和水淬爐石在不同溫度下與二氧化碳反應，脫硫渣重量變化遠高於水淬爐石，由XRD結果得知水淬爐石為非結晶固體在一定溫度下結構容易軟化，經研究發現在高溫下脫硫渣碳酸化反應遠優於水淬爐石。
3.在流體化床反應系統中，根據不同操作條件有溫度、水氣濃度、流速、二氧化碳濃度等參數。實驗結果發現二氧化碳濃度增加會使二氧化碳分壓提高而對爐渣的利用有顯著的影響；當氣體速度達到最小流化速度時，各種粒度的爐渣的利用率最好；而隨著提高流體化速度，爐渣利用率會隨之下降；在高溫下反應，在各種粒度的脫硫渣在5%的少量水氣濃度條件下可以促進二氧化碳捕獲。然而在各種粒徑的脫硫渣在10%的過量的水氣濃度條件下將會影響孔洞結構。
4.對於不同粒徑的脫硫渣在不同溫度下捕獲二氧化碳，發現其最佳溫度為600℃;對於不同粒徑的水淬爐石在不同溫度下捕獲二氧化碳，其最佳操作溫度為500℃。
5.以實驗室規模進行尺寸放大10倍的模場實驗，使用150-300μm粒徑的脫硫渣進行實驗，發現脫硫渣捕獲二氧化碳最佳溫度為600℃。因此在600℃下以脫硫渣進行從空氣和純氧燃燒條件下煙氣中捕獲二氧化碳。經由實驗結果發現純氧燃燒條件下脫硫渣捕獲二氧化碳的利用率高於空氣燃燒。

In recent years, fossil fuel has been widely used by human thus booming the economy. A great amount of carbon dioxide releasing from fossil fuel combustion causes the global warming. As a result, carbon dioxide capture and storage techniques are needed to solve this issue. Oxy-fuel combustion system is a carbon dioxide capture technology, contributing to higher capture efficiency due to concentrated CO2, decreasing processing cost, and easy alterations. This study used the water-quenched slag and the desulfurization slag as the sorbents. It not only reduces the cost of sorbent but also has a high calcium content that can highly absorb CO2 of the flue gas in a fluidized bed reactor system and increases the reutilization of the waste. Therefore, this study simulated oxy-fuel combustion condition to capture carbon dioxide with De-S and GGBS slags in a fluidized bed reactor system at high temperature.
Results of this study are summarized as follows：
1.With the increasing temperature both for empirical model prediction and experimental results, the minimum fluidized velocity of De-S and GGBS slags at various particle sizes have a decrease trend. However, the particle size and particle density of slags can influence the values of the minimum fluidized velocity at various temperatures.
2.According to the results of TGA analysis, De-S and GGBS slags react with carbon dioxide at various temperatures, weight change of the De-S slag is much higher than the GGBS slag.
3.Regarding to the various operating parameters such as temperature, water vapor, flow velocity and CO2 concentration, it can be found that an increase of the carbon dioxide concentration can significant impact the slags sorption utilization. When the gas velocity reaches minimum fluidized velocity, the sorption utilization sorption of the slags at various particle sizes will be the best. As the velocity becomes higher than minimum fluidized velocity, the slag sorption utilization decreases. The little water vapor for 5% can promote CO2 capture of slag at various particle sizes and excessive water vapor for 10% at various particle sizes affect pore structure.
4.The best operating temperature is about 600oC for the CO2 capture with De-S slag at various particle sizes; the best operating temperature is about 500oC for the CO2 capture with GGBS slag at various particle sizes. It can be found that De-S slags at various particle sizes for the CO2 capture are superior to the GGBS slags .
5.The pilot plant is 10 times the size of the laboratory set, conducting the capture of carbon dioxide from air and oxy-fuel combustion conditions. It can be found that the utilization of 150-300μm De-S slag at 600 oC is better than other temperature. The utilization of 150-300μm De-S slags for the capture of carbon dioxide from oxy-fuel combustion is higher than air combustion due to the increase in carbon dioxide partial pressure of the flue gas from oxy-fuel combustion.

摘要 I
Abstract III
致謝 V
Content VII
List of Figures XI
List of Tables XVI
Chapter 1Introduction 1
1-1Motivation 1
1-2Objectives 4
Chapter 2Literature Reviews 5
2-1Introduction to CO2 5
2-1.1Source 5
2-1.2Property 10
2-1.3Influence 12
2-2Principle of CO2 capture technique 16
2-2.1Absorption 18
2-2.2Cryogenic separation 22
2-2.3Membrane separation 23
2-3The positon for CO2 capture technique 24
2-3.1Post-combustion capture 24
2-3.2Pre-combustion capture 24
2-3.3Oxy-fuel combustion capture or O2 /CO2 combustion 25
2-3.4Comparison of carbon capture technologies 26
2-4Fluidized Bed 30
2-4.1Fluidization 30
2-4.2Minimum fluidized velocity 32
2-4.3Relationship between pressure drop and velocity 35
2-5Slag of Integrated Steel Work 37
2-5.1Ground-granulated blast furnaced and De-S slag 39
2-5.2Application of GGBS and De-S slag 40
2-6Activity decay of sorbent 42
2-7Influence of operating parameters 43
2-8Kinetics 45
2-8.1Deactivation model for the carbonation reaction 45
2-8.2Arrhenius equations 47
Chapter 3Methods and Materials 48
3-1Experimental methods 48
3-1.1Experimental design 48
3-1.2Experimental process 51
3-2Experimental equipments 52
3-2.1Experimental material 52
3-2.2Experimental facility 53
3-2.3Analyzers 60
3-3Preparation experiment 65
3-3.1Leakage proof of the system 65
3-3.2The slag preparation 65
3-3.3Span and zero 65
3-3.4Blank experiment 66
3-3.5Place the slag in the system 66
Chapter 4 Results and discussion 68
4-1Fluidization 70
4-1.1The relationship between pressure drop and superficial velocity 70
4-1.2The minimum fluidized velocity 73
4-2Characteristics of sorbents 79
4-2.1XRD analysis 79
4-2.2ICP-OES analysis 84
4-2.3TGA experiment 87
4-2.4BET surface area analysis 90
4-3Operating parameter experiment 93
4-3.1The De-S slag of 210-250μm 95
4-3.2The De-S slag of 177-210μm 99
4-3.3The GGBS slag of 210-250μm 103
4-3.4The GGBS slag of 177-210μm 106
4-4Characteristics of sorbents before and after carbonation 108
4-4.1SEM analysis 108
4-4.2EDS analysis 111
4-4.3Mapping analysis 116
4-4.4XPS analysis 121
4-4.5XRD analysis 124
4-5Pilot scale study 129
4-6Kinetics 135
Chapter 5Conclusions and suggestions 141
5-1Conclusions 141
5-2Suggestions 141
Chapter 6References 144
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