Hydrothermal Deactivation of Fe-ZSM-5 Prepared by Different Methods for the Selective Catalytic Reduction of NOx with NH3

doi:10.1016/S1872-2067(11)60326-4

Abstract

Abstract: A series of Fe/ZSM-5 catalysts were prepared by liquid ion exchange, incipient wetness impregnation, and solid-state ion exchange to investigate the selective catalytic reduction (SCR) of NO_x by NH₃(NH₃-SCR). The effect of hydrothermal deactivation of Fe-ZSM-5 catalysts prepared by different methods as a function of Fe loading was investigated. Freshly made and hydrothermal aged Fe-ZSM-5 catalysts were studied through NH₃-SCR activity test and characterized using X-ray diffraction, UV-Vis diffuse reflectance spectroscopy, and in situ diffuse reflectance infrared Fourier transform spectroscopy. Iron species on the surface of Fe-ZSM-5 catalysts were assigned to isolated Fe³⁺species, oligomeric Fe_xO_y clusters, and Fe₂O₃particles based on the UV-Vis spectra. The iron species distributions in the Fe-ZSM-5 catalysts prepared by these methods were quite different, which resulted in difference in SCR activity. The NH₃-SCR activity of different Fe-ZSM-5 catalysts became very similar after aging, and the activity of NH₃ oxidation and NO oxidation decreased with the aged catalysts. Characterization results indicated that the activity change of the aged Fe-ZSM-5 catalysts was due to the change of iron species distribution in Fe-ZSM-5 catalysts after hydrothermal aging. The relative concentration of isolated Fe³⁺species was decreased, whereas the relative concentration of oligomeric Fe_xO_y clusters and Fe₂O₃particles was increased in the aged catalysts. A considerable decrease in the Brønsted acidity of catalysts was observed for the aged Fe-ZSM-5 catalysts.

Key words: nitrogen oxide, selective catalytic reduction, iron, ZSM-5 zeolite, ammonia, hydrothermal aging

SHI Xiao-Yan, LIU Fu-Dong, DAN Wen-Po, HE Hong. Hydrothermal Deactivation of Fe-ZSM-5 Prepared by Different Methods for the Selective Catalytic Reduction of NO_x with NH₃[J]. Chinese Journal of Catalysis, 2012, 33(3): 454-464.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(11)60326-4

https://www.cjcatal.com/EN/Y2012/V33/I3/454

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Hydrothermal Deactivation of Fe-ZSM-5 Prepared by Different Methods for the Selective Catalytic Reduction of NO_x with NH₃

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