現在商業運轉之大型煤炭氣化複循環發電機組(IGCC)皆使用溼式商業化之除硫程序。然而溼式除硫必須用水來冷卻煤氣,使系統熱效率降低,為提高熱效率以降低發電及環保成本,世界各國皆在研發尋找高溫下乾式除硫方法。
本研究探討以自行製備之Mn2O3/γ-Al2O3吸著劑來吸收處理硫化氫，研究成果分成下列幾點探討:
1.比較負載於γ-Al2O3上之銅、錳、鋅、鈷、鐵、鈰系等六種吸著劑發現錳系及銅系吸著劑脫硫效能最好。
2.負載於不同載體之錳系吸著劑之脫硫效能以負載於γ-Al2O3之吸著劑脫硫效果最好,負載於SiO2之吸著劑脫硫效果次之,負載於TiO2之吸著劑脫硫效果最差。
3.以不同操作參數來觀察吸著劑利用率改變的情形,發現吸著劑利用率隨溫度升高、一氧化碳濃度增加、氫氣濃度減小而增加;而空間流速及硫化氫進流濃度則對吸著劑利用率無顯著之影響。
4.長期操作實驗部份,我們發現經過再生後再進行脫硫之吸著劑利用率明顯下降。由孔洞分析數據推論吸著劑再生後有燒結的情形。EDX分析顯示再生後之吸著劑內有硫元素存在,XPS圖譜進一步確認吸著劑中殘留之硫為硫酸根及亞硫酸根。最後在XRD圖譜中發現再生後之吸著劑只剩下γ-Al2O3特性波峰。
5.我們由動力研究發現,第一型衰退模式較符合實驗數據,所求得之活化能為86.9 KJ/mol。

Most large-scale existing commercial coal-based IGCC plants use wet scrubbers to remove H2S, but there are too much heat losses in the process. Therefore, it is necessary to find out a feasible dry desulfurization process operating under high temperature to raise the thermal efficiency and reduce the cost of the IGCC.
Desulfurization of hot syngas using homemade Mn2O3/γ-Al2O3 sorbent in a fixed bed reactor was conducted in this study. The explanation of results can be divided into five major parts.
1.The Zinc based sorbent and Copper based sorbent have the highest sorbent utilization among all the metal oxide sorbents supported on the γ-Al2O3 that we have tested.
2.The Manganese based sorbent supported on γ-Al2O3 has higher sorbent utilization than that supported on SiO2 and the Manganese based sorbent supported on TiO2 has the worst performance.
3.The effects of operating factors, such as inlet temperature, space velocity, CO inlet concentration, H2 inlet concentration and H2S inlet concentration on the absorption of H2S were performed. The results show that the sorbent utilization increases with the inlet temperature and CO concentration, and decreases as the H2 concentration increases. H2S concentration and space velocity, however, don’t change the sorbent utilization significantly.
4.The activity of the sorbent decreases significantly while sulfuration is operating after regeneration. Some instruments were employed to determine the characteristics of the sorbents after regeneration, such as BET, EDX, XPS, and XRD. From the results of pore analyses, we infer that sintering happens during regeneration. EDX spectra show that sulfur still exists in the sorbent after regeneration and we find that the forms of sulfur existed in the sorbent are sulfate and sulfite from XPS spectra. The peaks relating to Manganese disappear and only γ-Al2O3 can be identified in the XRD spectra of regenerated sorbents.
5.In the operating range of this study, we can find that Deactivation model typeⅠ is the most suitable model to fit the experimental data. We obtain the activity energy Ea=86.9 KJ/mole.

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