IrSn Bimetallic Clusters Confined in MFI Zeolites for CO Selective Catalytic Reduction of NOx in the Presence of Excess O2.

We developed a simple strategy for preparing IrSn bimetallic clusters encapsulated in pure silicon zeolites via a one-pot hydrothermal synthesis by using diethylamine as a stabilizing agent. A series of investigations verified that metal species have been confined successfully in the inner of MFI zeolites. IrSn bimetallic cluster catalysts were efficient for the CO selective catalytic reduction of NOx in the presence of excess O2. Furthermore, the 13CO temperature-programmed surface reaction results demonstrated that NO2 and N2O could form when most of the CO was transformed into CO2 and that Sn modification could passivate CO oxidation on the IrSn bimetallic clusters, leading to more reductants that could be used for NOx reduction at high temperatures. Furthermore, SO2 can also influence the NOx conversion by inhibiting the oxidation of CO. This study provides a new strategy for preparing efficient environmental catalysts with a high dispersion of metal species.

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.

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.

Preparation and Adsorption Properties of MCM-41 with Novel Gemini Ionic Liquid Surfactants as Template.

A mesoporous molecular sieve was prepared by the hydrothermal synthesis method with symmetric Gemini surfactant 1,3-bis(hexadecyldimethylammonio)-propane dibromide, symmetric Gemini ionic liquid surfactant 1,3-bis(3-hexadecylimidazolium-1-yl) propane dibromide and self-designed asymmetric Gemini ionic liquid surfactant 1-(3-(hexadecyldimethylammonio)prop-1-yl)-3-hexadecylimidazolium dibromide as the template agent. The structure characterization results for mesoporous molecular sieves show that the material possesses a hexagonal pore structure with uniform channels. The mesoporous silica that was synthesized with self-designed asymmetric Gemini ionic liquid surfactant as the template agent possesses the largest surface area and its pore size and specific surface area are, respectively, 3.28 nm and 879.37 m2/g. The adsorption properties of the prepared MCM-41 for crystal violet were investigated, and the adsorption thermodynamics and kinetics were investigated. The results show that adsorption equilibrium can be reached under pH = 9 and 35 °C for 50 min, and the quantity of adsorption can reach up to 464.21 mg/g. The adsorption process belongs to Langmuir isothermal adsorption, conforming to second-order adsorption kinetics, and the adsorption process is an endothermic process.

Structure-activity relationship and the inhibitory effect of sulfur dioxide and water on nitrous oxide formation in selective catalytic reduction of nitrogen oxides by ammonia over hollow Co3O4@CoMn2O4 catalyst.

Hollow structures have attracted great interest in many areas for their diverse applications. In this work, a new catalyst with an open and hollow structure (Co3O4@CoMn2O4) is designed for selective catalytic reduction of nitrogen oxides by ammonia (NH3-SCR). The as-prepared hollow-structured catalyst provides a high surface area and has thin shells. Owing to its structural benefits, this catalyst exhibited enhanced nitrogen oxides (NOx) removal activity and better resistance to water and sulfur dioxide than cobalt manganate nanoparticles. It also has proved that both the Eley-Rideal and Langmuir-Hinshelwood mechanisms are present in the NH3-SCR process in this catalyst. The improved nitrogen selectivity after the addition of water and sulfur dioxide occurs owing to the inhibition of nitrous oxide formation through the Eley-Rideal and Langmuir-Hinshelwood mechanisms. The deep insight into the structure-activity relationship and the influence of water and sulfur dioxide on nitrogen selectivity provide a new perspective for constructing high-performance de-NOx catalysts.