近年來人類大量使用化石燃料，使大氣中二氧化碳濃度不斷上升，造成嚴重的全球暖化以及全球氣候變遷等問題。因此，為了有效解決此問題，二氧化碳捕獲與封存技術是近年來非常受關注的議題。在這些技術中，化學環路燃燒 (Chemical looping combustion, CLC)被視為最有潛力且最具經濟效益之技術，可有效減少二氧化碳捕獲的成本，避免NOx生成，且增加燃燒效率。
本研究利用臨濕涵浸法自製Fe2O3/SiO2以及Fe2O3/Al2O3當成載氧體，於流體化床反應器與煤炭或生質體氣化合成氣 (H2, CO, CH4) 進行化學環路燃燒，探討不同操作條件 (氣體濃度、流體化速度、溫度)對載氧體利用率之影響。在TPR分析中，Fe2O3/SiO2和Fe2O3/Al2O3被氫氣還原使重量分別下降至原先的91.78 %以及90.59 %，根據其重量變化可知載氧體被還原至FeO與Fe之間。石英管實驗結果顯示濃度提高使擴散效果增加，能提升利用率，但CO和CH4濃度過高時會造成積碳現象；流速過高使停留時間太短，不利於反應。流速太低，載氧體無法流體化亦不利反應；溫度高達1,000℃時，燒結現象使利用率下降。當CH4 作為還原氣體與Fe2O3/Al2O3反應時，出現嚴重積碳現象。Fe2O3/SiO2經過10次循環反應及再生後，利用率下降至僅剩43%左右，可能是因為生成不可再生之Fe2SiO4尖晶石結構導致；Fe2O3/Al2O3則保持大約76% 的利用率。從XRD、XPS、FTIR、SEM的結果顯示，反應後之載氧體從Fe2O3晶像被還原至FeO與元素Fe之間，從XRD結果也確實發現Fe2O3/SiO2反應後會有Fe2SiO4晶像。當H2S加入系統後，由於其會與載氧體生成FeS結構，阻塞載氧體上之活性位置，導致載氧體與H2和CO反應的利用率下降。另外，從FTIR分析可知，H2S於系統中，與載氧體以及合成氣反應後最終將生成COS氣體。

In recent years, people have burned a great amount of fossil fuels, which dramatically increases the CO2 emission to the atmosphere. It causes some severe problems such as global warming and climate change. In order to solve the problems, carbon capture and storage (CCS) technologies become a great issue to reach the goals. Among these technologies, chemical looping combustion (CLC) has been considered as one of the most efficient and potential technologies which could effectively decrease the cost of CO2 capturing, avoid the formation of NOx and increase the combustion efficiency.
In this work, the incipient wetness impregnation method was used to prepare the Fe2O3/SiO2 and Fe2O3/Al2O3 oxygen carriers. The oxygen carriers were used to react with coal and biomass gasified syngas composed of H2, CO and CH4 under various operating parameters in order to investigate their influence to the utilization of oxygen carriers. In TPR analysis, the weight of Fe2O3/SiO2 and Fe2O3/Al2O3 are reduced to 91.78% and 90.59% by 10% H2, respectively. According to the weight loss, the oxygen carriers are reduced to the state between FeO and Fe. In tube test, results show that utilization of oxygen carriers would increase with concentration due to their higher diffusion capacity. However, there would be carbon deposition when CO and CH4 concentrations are too high. When the superficial velocity is too fast, the utilization would decrease due to short retention time. On the other hands, the utilization also decreases if the superficial velocity is too low which can’t generate a fluidized bed. As the temperature is up to 1,000℃, there would be agglomeration phenomena which cause a decrease of utilization. It is worth noting that there is a severe carbon masking problem for the CH4 test of Fe2O3/Al2O3. After 10 redox cycles, the utilization of Fe2O3/SiO2 dramatically decreases to about 43% due to the formation of Fe2SiO4 which can’t be fully reversible. However, Fe2O3/Al2O3 remains a good utilization at about 76% throughout the cycles. From the results of XRD, XPS, FTIR and SEM, Fe2O3 is indeed reduced to the state between FeO and Fe after combustion reaction. Besides, it is found that there is Fe2SiO4 structure after combustion reaction when SiO2 serves as the support. When H2S is added into the system, it would react with the oxygen carriers and form FeS structure which might block the active sites to cause a decrease of utilization. Furthermore, from the results of FTIR, H2S would react with the oxygen carriers and syngas, and ultimately transforms to COS.

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