Sulfation effect of Ce/TiO2 catalyst for the selective catalytic reduction of NO x with NH3: mechanism and kinetic studies

Ceria-based catalysts are competitive substitutes for the commercial SCR catalysts due to their high SCR activity and excellent redox performance. For a better understanding of the SO2 poisoning mechanism over ceria-based catalysts, the sulfation effect of the Ce/TiO2 catalyst on the SCR activity ov...

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Veröffentlicht in:RSC advances 2019-10, Vol.9 (55), p.32110
Hauptverfasser: Zhang, Wenjie, Liu, Guofu, Jiang, Jie, Tan, Yuchen, Wang, Qi, Gong, Chenghong, Shen, Dekui, Wu, Chunfei
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Sprache:eng
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Zusammenfassung:Ceria-based catalysts are competitive substitutes for the commercial SCR catalysts due to their high SCR activity and excellent redox performance. For a better understanding of the SO2 poisoning mechanism over ceria-based catalysts, the sulfation effect of the Ce/TiO2 catalyst on the SCR activity over a wide reaction temperature range was systematically studied via comprehensive characterizations, in situ DRIFT studies and kinetic studies. The results demonstrated that the NO conversion at 150 °C is significantly inhibited by the formation of cerium sulfites/sulfates due to the inhibited redox properties and excessive adsorption of NH3, which restrict the dissociation of NH3 to NH2, resulting in a much lower reaction rate of E-R reaction over the sulfated Ce/TiO2 catalyst. With the increase in the reaction temperature, the reaction rate of the E-R reaction significantly increased due to the improved redox properties and weakened adsorption of NH3. Moreover, the rate of the C-O reaction over the sulfated Ce/TiO2 catalysts is obviously lower than that of the fresh Ce/TiO2 catalyst. The promotion of NO conversion over the sulfated catalyst at 330 °C is attributed to both the increase in the reaction rate of E-R reaction and the inhibition of the C-O reaction.Ceria-based catalysts are competitive substitutes for the commercial SCR catalysts due to their high SCR activity and excellent redox performance. For a better understanding of the SO2 poisoning mechanism over ceria-based catalysts, the sulfation effect of the Ce/TiO2 catalyst on the SCR activity over a wide reaction temperature range was systematically studied via comprehensive characterizations, in situ DRIFT studies and kinetic studies. The results demonstrated that the NO conversion at 150 °C is significantly inhibited by the formation of cerium sulfites/sulfates due to the inhibited redox properties and excessive adsorption of NH3, which restrict the dissociation of NH3 to NH2, resulting in a much lower reaction rate of E-R reaction over the sulfated Ce/TiO2 catalyst. With the increase in the reaction temperature, the reaction rate of the E-R reaction significantly increased due to the improved redox properties and weakened adsorption of NH3. Moreover, the rate of the C-O reaction over the sulfated Ce/TiO2 catalysts is obviously lower than that of the fresh Ce/TiO2 catalyst. The promotion of NO conversion over the sulfated catalyst at 330 °C is attributed to both the increase in the reaction rate of
ISSN:2046-2069
2046-2069
DOI:10.1039/c9ra06985b