4.6 Article

Porous washcoat structure in CeO2 modified Cu-SSZ-13 monolith catalyst for NH3-SCR with improved catalytic performance

Journal

AICHE JOURNAL
Volume 68, Issue 11, Pages -

Publisher

WILEY
DOI: 10.1002/aic.17834

Keywords

low-temperature activity; mass transport; NH3-SCR; solvent combustion method; SSZ-13 zeolite

Funding

  1. Science and Technology Planning Project of Guangdong Province [2016B020241003]
  2. Natural Science Foundation of Guangdong Province [2018A030310563]

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CeO2 modified Cu-SSZ-13 monolith catalysts were prepared using the solvent combustion method, and the Ce2Cu-SSZ-13 catalyst showed excellent activity, stability and resistance in NH3-SCR of NO. The modification of CeO2 enhanced the acidity, redox capacity and ammonia adsorption capacity, leading to the high performance of Ce2Cu-SSZ-13 catalyst. In addition, the porous structure generated via solvent combustion increased the diffusion rate of reaction and the introduction of CeO2 promoted the oxidation of NO to NO2, resulting in fast SCR reaction.
A series of CeO2 modified Cu-SSZ-13 monolith catalysts were prepared by embedding CeO2 into the washcoat of Cu-SSZ-13 monolith catalyst through solvent combustion method. These CexCu-SSZ-13 catalysts were studied in the selective catalytic reduction (SCR) of NO with NH3, among which the Ce2Cu-SSZ-13 catalyst exhibited the best low-temperature activity, hydrothermal stability, and sulfur resistance. The physicochemical properties of the catalysts were characterized using multiple methods. Results showed that the acidity, redox capacity, and ammonia adsorption capacity significantly enhanced after CeO2 modification, thus leading to the high performance of Ce2Cu-SSZ-13 catalyst. Furthermore, the introduction of CeO2 induced the fast SCR reaction by promoting the oxidation of NO to NO2. Analog calculation suggested that the porous structure generated via solvent combustion in the washcoat effectively increased the diffusion rate of reaction. In situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFT) analysis showed that Bronsted acid sites were the main active center and the reaction followed Eley-Rideal mechanism.

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