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Effect of iron doping on SO2 and H2O resistance of honeycomb cordierite-based Mn–Ce/Al2O3 catalyst for NO removal at low temperature

Journal 2018 · IF 1.674 · 44(5): 3135-3150 · 发表于 2018 年 1 月 23 日
作者: Wang Cheng-zhi,Zhao Yong-gang,Zhang Cheng,Yan Xin,Cao Peng
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摘要

Honeycomb cordierite-based Mn–Ce/Al 2 O 3 (Mn–Ce/Al 2 O 3 –C) and Fe–Mn–Ce/Al 2 O 3 (Fe–Mn–Ce/Al 2 O 3 –C) catalysts were prepared by an impregnation method and investigated in low-temperature selective catalytic reduction (SCR) of NO with NH 3 at 100 °C. The Fe–Mn–Ce/Al 2 O 3 –C catalyst exhibited not only higher catalytic activity, but also much better SO 2 and H 2 O resistance in the presence of 30 ppm SO 2 and/or 5 vol% H 2 O than Mn–Ce/Al 2 O 3 –C. After doping Fe, the NO conversion of Mn–Ce/Al 2 O 3 –C catalyst displayed an increasing trend from 79 to 84% in the absence of SO 2 and H 2 O at 100 °C under a gas hour space velocity of 1667 h −1 . The results of characterization indicated that addition of Fe was advantageous to increase BET surface area, pore volume and inhibit loss of surface Mn and Ce species. Additionally, it was helpful for generating higher concentration of Mn 4+ , more chemisorbed oxygen and more uniform dispersion of amorphous Mn and Ce in the surface of catalyst, which were beneficial to interact with reactants. Furthermore, in contrast to Mn–Ce/Al 2 O 3 –C, the SCR activity of Fe–Mn–Ce/Al 2 O 3 –C catalyst in the presence of H 2 O, SO 2 and H 2 O and SO 2 were 79, 75 and 64%, with the increase of 14, 18 and 19%, respectively. It is indicated that the addition of Fe could inhibit sulfate formation and thus enhance SO 2 resistance. XPS results reveal that the doping of Fe into the ceria lattice led to some Ce 4+ transferred into Ce 3+ in order to maintain the electrical neutrality, thereby facilitating the reduction of Ce 4+  → Ce 3+ and the formation of oxygen vacancies. NH 3 temperature-programmed desorption (TPD) results imply that the doping of Fe onto Mn–Ce/Al 2 O 3 –C can remarkably improve the distribution and concentration of acid sites. All the above factors contributed to the improvement of overall NH 3 SCR performance of the Fe–Mn–Ce/Al 2 O 3 –C catalyst compared with that of the Mn–Ce/Al 2 O 3 –C catalyst.

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