工業革命後，人口快速成長、科技突飛猛進，進而大量使用化石燃料，溫室氣體之一的二氧化碳也因為大量化石燃料的燃燒而產生，累積在大氣中將造成溫度升高、海平面上升等全球氣候異常變遷，因此對二氧化碳進行有效的排放控制為當務之急。純氧燃燒系統具濃縮二氧化碳之特點，排放高濃度二氧化碳優點有提高捕獲效果、降低捕獲成本、易改建等，因此近期應用於化石燃料發電廠獲得高度重視。在二氧化碳捕獲技術中，可降低發電及環保成本之高溫乾式淨化系統是未來趨勢，且以鈣系爐石當作高溫固態吸收劑，可降低吸收劑成本與增加爐石再利用性，因此本實驗模擬純氧燃燒之煙道氣條件，以鈣系爐石（脫硫渣、氧化渣、還原渣與底渣）作為吸收劑，探討與二氧化碳在高溫下反應形成金屬碳酸鹽之研究。
本研究操作條件及研究成果分為下列幾部分說明：
1.由ICP和XRD分析結果顯示，脫硫渣的鈣氧化物含量（73.08%）明顯高於氧化渣（28.70%）、還原渣（39.34%）與底灰（2.00%），且脫硫渣中的Ca以Ca(OH)2形式存在，有利於碳酸化之反應。由TGA分析結果顯示，脫硫渣對CO2有較好的處理效果，其處理效果和爐石中鈣含量及其型式有顯著的關係。
2.以反應管模擬固定床，探討操作參數對脫硫渣吸收二氧化碳之實驗可以發現，溫度對脫硫渣吸收二氧化碳之最佳操作溫度為600oC；降低空間流速有助於碳酸化效果，但空間流速在1,200 mL hr-1 g-1~4,000 mL hr-1 g-1之間時利用率無顯著提升；添加水氣對脫硫渣碳酸化反應之影響，實驗結果發現水氣有助於碳酸化反應之利用率，當水氣濃度於5%時吸收效果最佳，之後隨著水氣濃度的增加，利用率有下降趨勢，推測水氣濃度過高，會使系統不平衡而阻礙碳酸化反應發生；二氧化硫的存在亦會降脫硫渣之利用率，提高二氧化硫之濃度，發現脫硫渣無法提供更多活性位置進行硫酸化反應。
3.利用XRD、SEM、FTIR作為輔助實驗進行反應前後脫硫渣吸收劑變化之分析。由XPS以及FTIR圖譜分析發現在水氣和二氧化硫同時存在下，經碳酸化反應後之產物除了以CaCO3的形式存在，並伴隨著硫化反應產生CaSO4。
4.由反應動力研究發現，第一型衰退模式所求得ko與kd之活化能分別為345.3 kJ/mol與13.4 kJ/mol，較合適用來描述本研究之動力模式。
5.本實驗亦以實驗室之固定床反應器結合工業燃燒爐，進行尺寸放大10倍，利用水淬高爐石為吸收劑，進行燃油與燃煤煙道氣現址二氧化碳捕捉與固定，研究發現水淬高爐石吸收二氧化碳之最佳操作溫度應為500oC，且水氣的存在與燃燒完全更有利於水淬高爐之碳酸化反應。

After industrial revolution, the increases of CO2 concentration in the atmosphere are resulted from the consumption of huge amounts of fossil fuels, and CO2 accumulating in the atmosphere will cause global climate changes including temperature increasing and ocean level rising. Hence, the effective control of CO2 emission is imperative. Oxyfuel combustion system is a CO2 concentrated technology, contributing to increasing capture efficiency, decreasing processing cost, and constructing easily. Recently, it is considered a new option for power generation. In CO2 capture technologies, the high temperature carbonation by dry techniques is a trend for related field. Calcium-based slags not only are used to absorb carbon dioxide but also reduce the cost of sorbents. In this study, the calcium-based slags (desulfurization slag, EAF oxidizing slag, EAF reductive slag and bottom ash) were used to absorb carbon dioxide in the simulated oxy-fuel combusted flue gas.
Results of this study are described as follows：
1.According to the results by using ICP and XRD analysis, the calcium oxide content of desulfurization slag (73.08%) is much higher than those of EAF furnace oxidizing slag (28.70%), EAF reductive slag (39.34%), and bottom ash (2.00%). Furthermore, the Ca form in desulfurization slag is Ca(OH)2, hence has a great potential on the carbonation. According to the results by using TGA analysis, desulfurization slag is the best choice in those slags for the removal of CO2, and the utilizaton is a function of calcium content of the slags.
2.In a fixed-bed reactor, the optimal operating temperature was about 600oC for the CO2 removal with desulfurization slag; the utilization ratio of the sorbent increased as the space velocity decreased before it was lower than 4,000 mL hr-1 g-1; the effects of adding water vapor on the carbonation of desulfurization slag were performed. The results indicate that the water vapor concentration can enhance the carbonation reaction and the optimal condition is 5%. However, the utilization decreases as the water vapor concentration increases over 5%, resulting from blocking of carbonation by extreme water vapor concentration. The effect of sulfur-containing flue gas shows that the overall utilization of the slag goes down, and the results are speculated that desulfurization slag could not provide more effective active sites to sulfurization.
3.The sorbents were examined for the better understanding of structure change, element composition and crystal transformation by XRD, SEM, FTIR. From the XPS and FTIR patterns, when the water vaper and SO2 existing simultaneously, the carbonated products contain not only CaCO3 but also CaSO4 because of the sulfurization.
4.For the kinetic study for the carbonation of desulfurization slag with experiment data at various temperatures, the first type of deactivation model is suitable to describe results.
5.In the study, carbon dioxide separation technology was also coupled with a oxy-coal combustion system, by using GGBF slag and the pilot plant located in NCKU Kuei-Len campus to demonstrate its feasibility in carbon dioxide sorption and look for the optimal operating conditions. Results of this study are described as follows (1)The optimal operating temperature is about 500°C for the carbon dioxide removal with GGBF slag. (2) The water vapor concentration and the higher degree of combustion completion can enhance the carbonation reaction.

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