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  • 學位論文

零價鐵/氧化鐵填充床結合一氧化碳處理氮氧化物/硫氧化物之研究

Simultaneous removal of Nitric Oxide and Sulfur Dioxide by Carbon Monoxide enhanced Zero Valent Iron/ Iron Oxide process

指導教授 : 陳孝行

摘要


本研究係利用市售微米級零價鐵粉(ZVI)、氧化鐵粉(α-Fe2O3)的混合鐵粉(Hybrid-Ferro)填充床反應器結合燃燒廢氣中之還原性氣體一氧化碳併同處理一氧化氮、二氧化硫之可行性研究,藉由改變四種操作參數,包括反應溫度、進流濃度、流通量、鐵粉量等,探討對一氧化氮、二氧化硫去除之影響。 從溫度效應方面,在溫度673K、723K、773K之填充床管柱實驗結果,反應溫度越高鐵粉的活性提升,能增加系統對NO、SO2的去除效率及操作時間,其累積鐵粉的NO、SO2去除量就越多。而隨進流濃度、流通量的提高,無論是NO或SO2與鐵粉接觸反應時,因參與反應之鐵粉較快消耗,使得去除率效果降低。在鐵粉量效應方面,NO、SO2、CO的去除效率及操作時間,均隨鐵粉量的增加而越好及延長,在混合鐵粉量(Fe、Fe2O3)的莫耳比例為0.5時,NO達反應終止之操作時間為SO2的1.6倍、CO的2.2倍;且在相同操作時間30min, NO、SO2、CO的平均去除率分別為93.49%、81.85%、63.72%。另以單一零價鐵粉、單一氧化鐵粉及混合鐵粉(0.5莫耳比例)對NO、SO2達反應終止時的累積鐵粉去除量而言,NO的去除量分別為6.2mg、0.2mg、15.5mg,SO2的去除量則分別為10.8mg、2.3mg、22.6mg,顯示以混合鐵粉對NO、SO2的累積去除量為最佳,其次為單一零價鐵粉,而單一氧化鐵粉的去除量為最差。 空床接觸時間(EBCT)與系統對NO、SO2、CO的操作時間之線性關係佳,應可作為填充床反應器之設計操作參數。將使用過鐵粉量經XRD試驗結果,其主要反應產物為FeS,Fe2O3或Fe3O4,因此我們可以推測其可能反應機制如下: 3Fe+2Fe2O3+2NO+2CO+SO2 → FeS+2Fe3O4+N2+2CO2 3Fe+Fe2O3+2NO+CO+SO2 → FeS+2Fe2O3+N2+CO2

並列摘要


This research project is a feasibility study of simultaneous removal of nitric oxide and sulfur dioxide by Hybrid-Ferro (mixing zero valent iron and iron oxide) packed bed reactor combined with reducing gas carbon monoxide. Several parameters were discussed, including reaction temperature, influent concentration, flux and dosage of Hybrid-Ferro. It is observed that with higher reaction temperature, the activity of Hybrid-Ferro and the removal efficiency of NO and SO2 were higher, and the operation time were also increased. The higher the flux, the lower the removal efficiency due to short contact time among Hybrid-Ferro, NO and SO2. Increased dosage for Hybrid-Ferro increased the removal efficiency and operation time of NO, SO2 and CO. For 773 K and 1 L/min, when the molar ratio of ZVI and α-Fe2O3 was 0.5, the operation time of NO was 1.6 times of SO2 and 2.2 times of CO. For operation time of 30 minutes, the average removal rates of NO, SO2 and CO were 93.5%, 81.9% and 63.7%, respectively. For 0.5 g (as Fe) of ZVI, α-Fe2O3 and Hybrid-Ferro (0.5 molar/each), mass of removed NO was 6.2 mg, 0.2 mg and 15.5 mg, and mass of removed SO2 was 10.8 mg, 2.3 mg, 22.6 mg, respectively. The experimentation shows removal efficiency for Hybrid-Ferro was best, and then ZVI and the worst was α-Fe2O3. Empty Bed Contact Time (EBCT) is linearly related to operation time of NO, SO2 and CO in this system; therefore, EBCT can be used as a design parameter for the packed bed. Used Hybrid-Ferro was tested by XRD and the presence of FeS、Fe2O3 and Fe2O3 were observed. According to the XRD test result, the following reactions are determined: 3Fe+2Fe2O3+2NO+2CO+SO2 → FeS+2Fe3O4+N2+2CO2 3Fe+Fe2O3+2NO+CO+SO2 → FeS+2Fe2O3+N2+CO2

參考文獻


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