Citation: Kai Qi, Junlin Xie, De Fang, Fengxiang Li, Feng He. Performance enhancement mechanism of Mn-based catalysts prepared under N₂ for NO_x removal: Evidence of the poor crystallization and oxidation of MnO_x[J]. Chinese Journal of Catalysis, ;2017, 38(5): 845-852. doi: 10.1016/S1872-2067(17)62814-6 shu

Performance enhancement mechanism of Mn-based catalysts prepared under N₂ for NO_x removal: Evidence of the poor crystallization and oxidation of MnO_x

Kai Qi ^a, ,
Junlin Xie ^a,b,c ,
De Fang ^a,b ,
Fengxiang Li ^a ,
Feng He ^a,c

a. State Key Laboratory of Silicate Materials for Architectures, Wuhan University of Technology, Wuhan 430070, Hubei, China;
b. Center for Materials Research and Test, Wuhan University of Technology, Wuhan 430070, Hubei, China;
c. School of Materials Science and Engineering, Wuhan University of Technology, Wuhan 430070, Hubei, China

Received Date: 9 February 2017
Revised Date: 10 March 2017

Among multitudinous metal-oxide catalysts for the selective catalytic reduction of NO_x with NH₃ (NH₃-SCR), Mn-based catalysts have become very popular and developed rapidly in recent years because of its superior low-temperature denitrification activity, mainly originating from multi-valence of Mn. Most studies suggest that the catalytic activity of multi-component oxides is superior to that of single-component catalysts owing to the synergistic effect among the metallic elements in such materials, of which more attentions have been given to Ce as an additive owing to its powerful oxygen storage capacity, redox ability and its ready availability. As the core of SCR technology, the research points in catalyst development at the present stage of all researchers in countries mainly centralize on the optimization of active components, carriers, calcination temperature, calcination time and temperature-raising procedure, giving little thought to the effects of the calcination atmosphere. In the present work, Ce-modified Mn-based catalysts were prepared by a simple impregnation method. The effects of the calcination atmosphere (N₂, air or O₂) on the performance of the resulting materials during NH₃-SCR and its causes of the differences were subsequently investigated and characterized using various analytical methods. Data obtained from X-ray diffraction, thermogravimetry and temperature-programmed reduction with hydrogen show that calcination under N₂ reduces both the degree of oxidation and crystallization of the MnO_x. Scanning electron microscopy also demonstrates that the use of N₂ inhibits the growth of grains and increases the dispersion of the catalysts. In addition, the results of temperature-programmed desorption with ammonia indicate that catalysts calcined under N₂ exhibit a greater quantity of acid sites. Finally, X-ray photoelectron spectrometry and activity results demonstrate that MnO_x in the lower valence states is more favorable for NH₃-SCR reactions. In conclusion, catalysts calcined under N₂ show superior performance during NH₃-SCR for NO_x removal, allowing NO conversions up to 94% at 473 K.
- Mn-based catalyst,
- Selective catalytic reduction,
- Calcination atmosphere,
- Mn species,
- Oxidation degree,
- Crystallization degree
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Performance enhancement mechanism of Mn-based catalysts prepared under N2 for NOx removal: Evidence of the poor crystallization and oxidation of MnOx

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通讯作者: 陈斌, bchen63@163.com

Performance enhancement mechanism of Mn-based catalysts prepared under N₂ for NO_x removal: Evidence of the poor crystallization and oxidation of MnO_x