“NO2 SCR”对Mn、Ce基脱硝催化剂超低温性能提高及其吸附机理研究

Study on the improvement of ultra-low temperature performance and adsorption mechanism of Mn and Ce based denitrification catalysts by "NO2 SCR

  • 摘要: 用共沉淀法制备的Mn7Fe4Ce9Ox/AlOx和 Mn3Fe1Ce6Ox/AlOx负载催化剂,在7777 h−1进气条件下发生标准SCR机理反应进行评价,两种催化剂在60 ℃只有10%左右的催化活性,在相同条件下增加进气中的NO2/NOx浓度比例,以0、14.3%、28.6%、42.8%、57%、71.4%、85.7%、100%的进气NO2/NOx浓度比例再进行评价,结果表明,Mn3Fe1Ce6Ox/AlOx催化剂在60 ℃可以有64%的脱硝效率,相比首次评价提升了58%左右。实验和理论计算表明,Mn3Fe1Ce6Ox/AlOx催化剂有更大的比表面积、更强的NO2吸附和活化,从而提高了NO2快速SCR机制反应的效率。同时在原位红外测试中发现,增加NO2/NOx浓度比例时Mn3Fe1Ce6Ox/AlOx催化剂吸附方式出现了明显地变化,催化剂由NH3吸附为主的E-R和L-H机理变为以NO2吸附为主的E-R和L-H机理,吸附机理的变化是催化剂在超低温性能提高的关键因素。这项工作为探究高效经济地NH3-SCR脱硝提供一种很有前景的策略,同时也为超低温烟气处理提供经验,以及烟气处理新工艺提供指导。

     

    Abstract: The catalysts supported by Mn7Fe4Ce9Ox/AlOx and Mn3Fe1Ce6Ox/AlOx prepared by co-precipitation method were first evaluated by standard SCR mechanism reaction under 7777 h−1 intake condition. The catalytic activity of the two catalysts was only about 10% at 60 ℃. Then, the concentration ratio of NO2/NOx in intake air was increased under the same conditions, and the concentration ratio of NO2/NOx in intake air was 0%, 14.3%, 28.6%, 42.8%, 57%, 71.4%, 85.7% and 100%. The results show that the denitrification efficiency of Mn3Fe1Ce6Ox/AlOx catalyst can be 64% at 60 ℃, which is about 58% higher than that of the first evaluation. Experimental and theoretical calculations show that Mn3Fe1Ce6Ox/AlOx catalyst has larger specific surface area and stronger adsorption and activation of NO2, which improves the efficiency of NO2 fast SCR mechanism reaction. At the same time, the in situ infrared test found that the adsorption mode of Mn3Fe1Ce6Ox/AlOx catalyst changed significantly when the concentration ratio of NO2/NOx increased, and the E-R and L-H mechanism mainly adsorbed by NH3 changed to the E-R and L-H mechanism mainly adsorbed by NO2. The change of adsorption mechanism may be the key factor to improve the performance of catalyst at ultra-low temperature. This work provides a promising strategy for exploring efficient and economical denitrification of NH3-SCR, as well as experience for ultra-low temperature flue gas treatment and guidance for new flue gas treatment processes.

     

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