4.6 Article

The deactivation mechanism of Pb on the Ce/TiO2 catalyst for the selective catalytic reduction of NOx with NH3: TPD and DRIFT studies

Journal

PHYSICAL CHEMISTRY CHEMICAL PHYSICS
Volume 19, Issue 7, Pages 5333-5342

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/c6cp07271b

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Funding

  1. Natural Science Foundation of China [21546014]
  2. Natural Science Foundation of Shanghai, China [14ZR1417800]

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It was well recognized that Pb had a poisoning effect on a SCR catalyst. In this study, the deactivation mechanism of Pb on the Ce/TiO2 catalyst was investigated based on the characterization results of TPD and in situ DRIFT studies. It was found that the addition of Pb on the Ce/TiO2 catalyst not only inhibited the adsorption and activation of NH3 species, but also led to the decrease of the activity of adsorbed NH3 species in the SCR reaction. The adsorption of NOx species and the oxidation of NO by O-2 over the Ce/TiO2 catalyst were also suppressed by the addition of Pb, while the reactivity of adsorbed NO2 species did not decrease. Moreover, the results revealed that the NH3-SCR reaction over the Ce/TiO2 catalyst followed both the E-R and L-H mechanisms, while the NH3-SCR reaction over Ce/TiO2-Pb was mainly controlled by the L-H mechanism. The contributions of the L-H mechanism to the SCR reactions over Ce/TiO2 and Ce/TiO2-Pb decreased with increasing reaction temperature. The deactivation of Ce/TiO2-Pb was mainly attributed to the suppressed NH3 adsorption and activation, accompanied by the inhibited NO oxidation and the decrease of Bronsted acid sites.

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