Effects of adsorbed and gaseous NOx species on catalytic oxidation of diesel soot with MnOx–CeO2 mixed oxides

Abstract

MnOx–CeO2, MnOx and CeO2 catalysts were synthesized by the sol–gel method. The structural, redox and adsorption properties of the individual and mixed oxides were investigated by X-ray diffraction (XRD), Brunauer–Emmett–Teller (BET), CO temperature-programmed reduction (TPR), NO temperature-programmed oxidation (TPO), NOx temperature-programmed desorption (TPD) and in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). The TPO tests were performed with the soot–catalyst mixture under loose contact conditions to evaluate the catalytic activity of the oxide catalysts for soot oxidation. The MnOx–CeO2 mixed oxide catalyst presents the lowest soot oxidation temperature among the catalysts investigated in the presence of NO and O2. The synergetic effect between manganese oxide and ceria restrains the growth of oxide crystallites, increases the specific surface area and improves the low-temperature redox property. Especially, the activity of MnOx–CeO2 mixed oxides for NO oxidation and its capacity for NO2 storage in the form of surface nitrates are greatly enhanced. Not only the NO2 released from decomposition of surface nitrates but also that formed by catalytic oxidation of gaseous or adsorbed NO on the catalyst is confirmed important for soot oxidation. It is found by the in situ DRIFTS tests with the soot–catalyst mixture that the generation of surface oxygen complexes (SOCs), such as carboxylic anhydrides, lactones, quinine, ceto-enol groups, ethers and phenols, occurs at about 100°C lower temperature with exposure to NO than in the absence of NO, which is an important step for soot oxidation.