ABSTRACT
Recently, ozone pollution has gradually replaced PM2.5 as the main pollutant affecting air pollution. In this study, we synthesized a series of Mn3O4 catalysts by hydrothermal method changing the precursors and tested their activities at different relative humidity, gas volume space velocity of 150,000 h-1 and 5 ppm ozone. Remarkably, Mn3O4-SO4 prepared with MnSO4 as precursor showed excellent catalytic ozone decomposition activity, almost completely converting 5 ppm of ozone at different relative humidity ranges. Finally, the most active Mn3O4-SO4 catalyst was tested for its usability limit at RH= 90%, after 28 h of testing under high humidity conditions, it had retained successfully the complete decomposition of low concentrations of ozone. The catalysts were characterized by XRD, Raman, HRTEM, XPS, BET, H2O-TPD and in situ IR NH3 adsorption. The characterization analysis revealed that the Mn3O4-SO4 surface could exposed a highly active (101) crystalline surface with high specific surface area, excellent hydrophobicity as well as ozone adsorption capacity, which were highly favorable for ozone decomposition under high humidity conditions. In this work, Mn3O4 exhibits good catalytic activity, which provides an additional option for future studies of manganese oxides.
ABSTRACT
The hydrothermal stability of NO oxidation is the key to the practical application of diesel oxidation catalysts in diesel engines, which in the laboratory requires that NO activity does not decrease after aging for 10 h with 10% H2O/air at 800 °C. On the one hand, the construction of a metal/oxide interface can lead to abundant oxygen vacancies (Ov), which compensate for the loss of activity caused by the aggregation of Pt particles after aging. On the other hand, YMn2O5 (YMO) has excellent thermal stability and NO oxidation capacity. Therefore, a Pt/YMn2O5-La-Al2O3 (Pt/YMO-LA) catalyst was prepared by the impregnation method. The support of the catalyst, YMn2O5-La-Al2O3 (YMO-LA), was obtained by mixing high specific surface LA and YMO ball-milling. Under laboratory-simulated diesel exhaust flow, the NO oxidation performance of Pt/YMO-LA did not decrease after hydrothermal aging. Combining high-resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectroscopy (XPS), and oxygen temperature-programmed desorption (O2-TPD), the Pt/YMn2O5 interface was formed after hydrothermal aging, and the increased Ov can provide reactive oxygen to Pt and YMO. The cooperative catalysis of multiple active centers composed of Pt, YMO, and Ov is the crucial factor to maintain the NO oxidation performance. In addition, in situ diffuse reflectance infrared Fourier transform spectra (DRIFTs) show that an increase in Ov is beneficial to the adsorption and desorption of more nitrate and nitrite intermediates, thus achieving the hydrothermal stability of NO oxidation.
ABSTRACT
Eliminating vehicle emission is of importance due to the severe limit value. The work reports a convenient strategy of improving dispersion of platinum-based catalyst with the assistance of polyvinyl alcohol in a varied addition amount. Following the "two-step" annealing techniques, the catalytic performance of the polymer-assisted catalysts in diesel was obviously enhanced because of the improved dispersion of the platinum. Based on experimental results, the long chains of polymer resulting in the steric effect are presumed to isolate platinum ion, inhibiting the aggregation of platinum particles and then improving its dispersion. And the hydroxyl bonding between the polymers could convey electron to platinum species, leading to the lower platinum valence state. Both effects are positive resulting in an excellent NO maximum conversion of around 65% at the optimal introduction of 5 mass% of polymer, as the diesel oxidation catalyst (DOC), which could be inclined to a good purification in the diesel aftertreatment. Hopefully, the convenient research method could initiate the exploration and application of polymer-assisted catalysts for well-dispersed noble metal nanoparticles in eliminating exhaust emission.
