Removal of NOx and soot over Ce/Zr/K/Me (Me = Fe, Pt, Ru, Au) oxide catalysts

Abstract

The potentiality of ceria/zirconia based catalysts in the simultaneous removal of particulate matter (soot) and NOx is investigated in this work, and compared with that of a model LNT Pt-K/Al2O3 sample. Ceria-zirconia (molar ratio 75/25) catalysts doped with Pt, Au, Ru or Fe (2% by weight) and containing K (7% by weight) were prepared by a modified citrate method and characterized by X-ray diffraction, surface area and pore volume measurements. The behavior of the catalysts in the soot combustion and NOx removal was separately analyzed by means of temperature programmed oxidation (TPO), isothermal combustion and isothermal NOx adsorption experiments. The results showed that all the ceria/zirconia based catalysts are more active than Pt-K/Al2O3 in soot combustion; the Ru-containing system also showed NOx storage performances comparable to Pt-K/Al2O3. Accordingly the capability of the Ru-based catalyst to accomplish the removal of NOx in the absence and in the presence of soot was further investigated by reactivity experiments and FT-IR spectroscopy to analyze both the gas phase and the catalyst surface species. The data indicate that the Ru-based system is able to simultaneously remove soot and adsorb NOx pointing out higher performances in the soot combustion as compared to the Pt-K/Al2O3 catalyst, and similar behavior in the NOx storage capacity. However the NOx reduction activity results lower than the traditional LNT Pt-based catalyst. Conversely, when the Ru-based catalyst is mixed with the LNT sample (physical mixture) a NOx reduction efficiency similar to Pt-K/Al2O3 is found.