Improved NO x Reduction in the Presence of SO2 by Using Fe2O3-Promoted Halloysite-Supported CeO2-WO3 Catalysts.

Currently, selective catalytic reduction (SCR) of NO x with NH3 in the presence of SO2 by using vanadium-free catalysts is still an important issue for the removal of NO x for stationary sources. Developing high-performance catalysts for NO x reduction in the presence of SO2 is a significant challenge. In this work, a series of Fe2O3-promoted halloysite-supported CeO2-WO3 catalysts were synthesized by a molten salt treatment followed by the impregnation method and demonstrated improved NO x reduction in the presence of SO2. The obtained catalyst exhibits superior catalytic activity, high N2 selectivity over a wide temperature range from 270 to 420 °C, and excellent sulfur-poisoning resistance. It has been demonstrated that the Fe2O3-promoted halloysite-supported CeO2-WO3 catalyst increased the ratio of Ce3+ and the amount of surface oxygen vacancies and enhanced the interaction between active components. Moreover, the SCR reaction mechanism of the obtained catalyst was studied using in situ diffuse reflectance infrared Fourier transform spectroscopy. It can be inferred that the number of Brønsted acid sites is significantly increased, and more active species could be produced by Fe2O3 promotion. Furthermore, in the presence of SO2, the Fe2O3-promoted halloysite-supported CeO2-WO3 catalyst can effectively prevent the irreversible bonding of SO2 with the active components, making the catalyst exhibit desirable sulfur resistance. The work paves the way for the development of high-performance SCR catalysts with improved NO x reduction in the presence of SO2.

Design of meso-TiO2@MnO(x)-CeO(x)/CNTs with a core-shell structure as DeNO(x) catalysts: promotion of activity, stability and SO2-tolerance.

Developing low-temperature deNOx catalysts with high catalytic activity, SO2-tolerance and stability is highly desirable but remains challenging. Herein, by coating the mesoporous TiO2 layers on carbon nanotubes (CNTs)-supported MnOx and CeOx nanoparticles (NPs), we obtained a core-shell structural deNOx catalyst with high catalytic activity, good SO2-tolerance and enhanced stability. Transmission electron microscopy, X-ray diffraction, N2 sorption, X-ray photoelectron spectroscopy, H2 temperature-programmed reduction and NH3 temperature-programmed desorption have been used to elucidate the structure and surface properties of the obtained catalysts. Both the specific surface area and chemisorbed oxygen species are enhanced by the coating of meso-TiO2 sheaths. The meso-TiO2 sheaths not only enhance the acid strength but also raise acid amounts. Moreover, there is a strong interaction among the manganese oxide, cerium oxide and meso-TiO2 sheaths. Based on these favorable properties, the meso-TiO2 coated catalyst exhibits a higher activity and more extensive operating-temperature window, compared to the uncoated catalyst. In addition, the meso-TiO2 sheaths can serve as an effective barrier to prevent the aggregation of metal oxide NPs during stability testing. As a result, the meso-TiO2 overcoated catalyst exhibits a much better stability than the uncoated one. More importantly, the meso-TiO2 sheaths can not only prevent the generation of ammonium sulfate species from blocking the active sites but also inhibit the formation of manganese sulfate, resulting in a higher SO2-tolerance. These results indicate that the design of a core-shell structure is effective to promote the performance of deNOx catalysts.