二氧化碳是目前地球大氣中最重要的人為溫室氣體，伴隨著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。純氧燃燒系統是一種二氧化碳濃集技術，排放之高濃度二氧化碳有提高捕獲效果、降低捕獲成本、易改建等優勢，近期應用於化石燃料發電廠獲得高度重視。二氧化碳捕獲技術中，可降低發電成本之高溫乾式淨化系統是未來趨勢，再加上矽酸鋰被視為最有前瞻性之高溫固態吸收劑之一，因此，本研究模擬純氧燃煤之煙道氣條件，以自製矽酸鋰作為吸收劑去除二氧化碳之研究。
　　本研究以溶膠凝膠法製備矽酸鋰吸收劑，透過X射線繞射儀(XRD)、熱重分析儀(TGA)探討鍛燒程序之影響，得知鍛燒溫度與鍛燒時間分別為700oC及5hr之矽酸鋰結晶構造較純且有較佳之碳酸化效果(88%)，因此選定此鍛燒條件以確立製備程序。以反應管模擬固定床，探討操作參數對矽酸鋰去除二氧化碳之實驗可以發現，降低空間流速有助於碳酸化效果，空間流速低於6,000 mL hr-1 g-1時，利用率無顯著提升，相差5%以內；溫度對自製矽酸鋰去除二氧化碳之最佳操作溫度應為700oC左右；水氣參與碳酸化反應對吸收劑之影響，實驗結果可得水氣會降低矽酸鋰之利用率，當水氣濃度大於10%，利用率下降一半以上，推測水氣的存在阻擋活性位置與二氧化碳之反應，導致矽酸鋰利用率顯著降低；二氧化硫的存在亦會降低矽酸鋰之利用率，然而提高二氧化硫之濃度，發現矽酸鋰之利用率有停滯的現象，推測矽酸鋰無法提供更多活性位置進行硫酸化反應。
　　本文利用XRD、SEM、XPS、FTIR作為輔助實驗進行反應前後矽酸鋰吸收劑變化之分析。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Li2SiO3與Li2CO3的形式存在，並伴隨著硫化反應產生Li2SO4。且由動力研究發現，第一型衰退模式較適合用來描述此結果，自製矽酸鋰活化能Ea = 51.5 kJ/mol，碰撞因子A = 1.7 × 1013。

　　Carbon dioxide is the most important anthropogenic greenhouse gases in the atmosphere, accompanied by huge amounts of fossil fuels combustion. 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, and Li4SiO4 is considered a promising sorbent for removing CO2. In the present work, the handmade Li4SiO4 sorbent was used for the capture of carbon dioxide in the simulated oxy-fuel combusted flue gas.
　　To establish synthesized method, Lithium orthosilicate sorbent was synthesized by sol-gel method and was investigated for the effects of calcination by XRD and TGA. The suitable condition of the sorbent was calcined at 700oC for 5 hours because of the high purity of crystal structure and great carbonated reactivity (88%). In a fixed-bed reactor, the utilization ratio of the sorbent increased as the space velocity decreased before it was lower than 6,000 mL hr-1 g-1; the optimal operating temperature was about 700oC; the effects of adding water vapor on the carbonation of Li4SiO4 were performed. The results indicate that the utilization decreased with increasing water vapor concentration. As the water vapor concentration greater than 10%, the utilization is decreased by half or more. The existence of stream could mask the active sites of sorbent, so consequently the utilization ratio decreased; the effect of Li4SiO4 sorbent in sulfure-containing flue gas showed that the overall utilization went down. However, when increasing the SO2 concentration, the utilization has the phenomenon of stagnation. The results were speculated that Li4SiO4 sorbent couldn’t provide more effective active sites to sulfurization.
　　The sorbents will be examined for the better understanding of structure change, element composition and crystal transformation by XRD, SEM, XPS, FTIR. From the XPS and FTIR patterns, when the water vaper and H2S existing simultaneously, the carbonated production contains not only Li2SiO3 and Li2SiO3 but also Li2SO4 because of the sulfurization. The kinetic model for the carbonation of Li4SiO4 sorbent with different temperatures of experiment results, the first deactivation model is suitable to describe results.

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