Tailoring Iridium Valence States on ZSM-5 for Enhanced Catalytic Performance in CO Selective Catalytic Reduction of NO under Oxygen-Enriched Environments.

Barium and iridium supported on Zeolite Socony Mobil-5 (ZSM-5) are efficient catalysts for the selective catalytic reduction of nitric oxide by carbon monoxide (CO-SCR), with enhanced cyclic stability. The introduction of Ba hindered the oxidation of metallic Ir active species and enabled Ir to maintain an active metallic state, thereby preventing a decrease in catalytic activity in the CO-SCR reaction. Moreover, the Ba modification increased the NO adsorption of the catalyst, further improving the catalytic activity. Owing to the better anti-oxidation ability of Ir0 in IrBa0.2/ZSM-5(27) than in Ir/ZSM-5(27), IrBa0.2/ZSM-5(27) showed better stability than Ir/ZSM-5(27). Considering that all samples in the present study were tested to simulate actual flue gases (such as sintering flue gas and coke oven flue gas), NH3 was introduced into the reaction system to serve as an extra reductant for NOx. The NOx conversion to N2 (77.1%) was substantially improved using the NH3-CO-SCR system. The proposed catalysts and reaction systems are promising alternatives for treating flue gas, which contains considerable amounts of NOx and CO in oxygen-enriched environments.

Insight into the Mechanism of Selective Catalytic Reduction of NO by CO over a Bimetallic IrRu/ZSM-5 Catalyst in the Absence/Presence of O2 by Isotopic C13O Tracing Methods.

The development of efficient catalysts for the selective catalytic reduction of NO by CO (CO-SCR) in the presence of O2 is highly desirable for controlling the emission of toxic gases from tailpipes. Here, a bimetallic IrRu/ZSM-5 catalyst was prepared for the selective catalytic reduction of NO by CO in the presence of O2 (5%) for the low-temperature treatment of exhaust gas. IrRu/ZSM-5 afforded 90% NOx conversion in the range of 225-250 °C and maintained 90% NOx conversion after 12 h of reaction. Ru addition inhibited agglomeration of the Ir particles during the reduction process and provided more active sites for NO adsorption. Isotopic C13O tracing and in situ diffuse reflectance infrared Fourier-transform spectroscopy experiments were used to elucidate the CO-SCR mechanism in the absence or presence of O2. NCO could easily form on the surface of catalysts in the absence of O2, whereas NCO formation has been inhibited owing to the quick consumption of CO in the presence of O2. Moreover, some byproducts such as N2O and NO2 are generated in the presence of O2. Finally, a possible mechanism for CO-SCR under different conditions was proposed based on in situ experiments and physicochemical analyses.

Simultaneous removal of NO and dichloromethane (CH2Cl2) over Nb-loaded cerium nanotubes catalyst.

Herein, a series of niobium oxide supported cerium nanotubes (CeNTs) catalysts with different loading amount of Nb2O5 (0-10 wt.%) were prepared and used for selective catalytic reduction of NOx with NH3 (NH3-SCR) in the presence of CH2Cl2. Commercial V2O5-WO3-TiO2 catalyst was also prepared for comparison. The physcial properties and chemical properties of the Nb2O5 loaded cerium nanotubes catalysts were investigated by X-ray diffractometer, Transmission electron microscope, Brunauer-Emmett-Teller specific surface area, H2-temperature programmed reduction, NH3-temperature programmed desorption and X-ray photoelectron spectroscopy. The experiment results showed that the loading amount of Nb2O5 had a significant effect on the catalytic performance of the catalysts. 10 wt.% Nb-CeNTs catalyst presented the best NH3-SCR performance and degradation efficiency of CH2Cl2 among the prepared catalysts, due to its superior redox capability, abundant surface oxygen species and acid sites, the interaction between Nb and Ce, higher ratio of Nb4+/(Nb5++ Nb4+) and Ce3+/(Ce3+ + Ce4+), as well as the special tubular structure of cerium nanotube. This study may provide a practical approach for the design and synthesis of SCR catalysts for the simultaneously removal NOx and chlorinated volatile organic compounds (CVOCs) emitted from the stationary industrial sources.

Effect of Cr doping in promoting the catalytic oxidation of dichloromethane (CH2Cl2) over Cr-Co@Z catalysts.

A core-shell catalyst which consists of a Co3O4 core and ZSM-5 shell, was prepared by microwave hydrothermal method and subjected for dichloromethane (DCM) oxidation. Chromium, cerium, niobium, and manganese species were separately introduced into the core-shell catalyst using the wet precipitation method and denoted as M-Co@Z (M = Cr, Ce, Nb, Mn). The catalytic activity of the Cr-Co@Z catalyst was significantly increased due to the interaction between Cr2O3 and Co3O4. The results of Raman spectra indicated the incorporation of chromium into the Co3O4 lattice and revealed the existence of the interaction between Cr2O3 and Co3O4. The synergistic effect between Cr2O3 and Co3O4 might be conducive to the generation of highly defective structure and increase the ratio of Co3+/Co2+ of the sample, leading to its better oxygen mobility. The dechlorination ability of Cr-Co@Z was also promoted due to the enhanced mobility of lattice oxygen. Based on in situ DRIFT studies, a possible reaction route of CH2Cl2 oxidation over Cr-Co@Z catalyst was proposed.