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.

Preventing emission of pollutants in any kind, is a way to protect global environment. The objective of this study is to develop cobalt catalysts supported on alumina for the conversion of the toxic gas SO2 into elemental sulfur using methane. Although several useful catalysts have been proposed, there is still a need to synthesize a catalyst with a high sulfur yield that is also persistent during on-stream stability. To this end, four different catalysts were prepared using the wet impregnation technique, with Co3O4 content ranging from 0 to 15 wt%. Catalytic activity tests were carried out at atmospheric pressure and temperatures ranging from 550 to 800 °C. The Al2O3-Co (15 %) catalyst exhibited superior performance, with a sulfur yield of 98.1 % at 750 °C. The catalytic stability of the best catalyst was examined using a 20 h on-stream stability test under the optimized conditions including an SO2/CH4 molar feed ratio of 2 at 750 °C. The structural changes of the used catalyst after the stability test were investigated using XRD and TPO analyses. It was revealed that sulfidation of Co3O4 after a short while, results in decreasing the sulfur yield from 98.1 % to 89.8 %.

An iterative approach between machine learning (ML) and laboratory experiments was developed to accelerate the design and synthesis of environmental catalysts (ECs) using selective catalytic reduction (SCR) of nitrogen oxides (NOx) as an example. The main steps in the approach include training a ML model using the relevant data collected from the literature, screening candidate catalysts from the trained model, experimentally synthesizing and characterizing the candidates, updating the ML model by incorporating the new experimental results, and screening promising catalysts again with the updated model. This process is iterated with a goal to obtain an optimized catalyst. Using the iterative approach in this study, a novel SCR NOx catalyst with low cost, high activity, and a wide range of application temperatures was found and successfully synthesized after four iterations. The approach is general enough that it can be readily extended for screening and optimizing the design of other environmental catalysts and has strong implications for the discovery of other environmental materials.

Based on the unique technique property of grate-kiln pellet production process and its demand of ultra-low emission of NOx, a low energy-consumed embedded selective catalytic reduction (SCR) denitration technology was proposed. The temperature of the NOx-containing tributary flue gas was 350-500 °C, which basically accorded with the temperature range of SCR by V2O5-based catalyst. Considering the potential inhibition effect of high SO2 concentration (8000-10000 mg/m3) and metal-containing dust in the pelletizing flue gas, the catalyst compositions were optimized to V2O5 (0.5%) and WO3 (5%), giving NO conversion over 90% with low yield of N2O by-product. Compared with the low-medium temperature SCR technology, it was no longer necessary to reheat the flue gas, showing a remarkable CO2 emission reduction effect. The CO2 emission reduction ratios were 94% and 66% contributed by the decrease of fuel and electricity consumption for the embedded SCR technology, respectively. The operating cost was also greatly reduced from 11.4 CNY/t-pellet to 3.1 CNY/t-pellet (Chinese Yuan).

This work prepared an ISAPO-34/SAPO-18 intergrown zeolite using phosphate organoamine as the structure guiding agent. Physical-chemical characterizations by XRD, SEM, TG, and BET showed that the SAPO-34/SAPO-18 presents a cross-stacked cubic block-like microscopic morphology, with characteristic diffusive diffraction peaks at 2θ = 16-18° and 30-33° and a specific surface area of 557 m2 g-1. The series of copper-based catalysts prepared from SAPO-34/SAPO-18 showed a shift of the active temperature window to a lower temperature with increasing copper content. Moreover, the Brønsted acid site decreased significantly due to copper ion exchange and zeolite structure framework damage. Among them, the 1.2 wt% sample showed the widest active temperature window, with a T90 range of 175-435°C. After low-temperature hydrothermal aging treatment, the zeolite structure was eroded and the catalyst activity deteriorated significantly.

Developing low-temperature SO2-tolerant catalysts for the selective catalytic reduction of NOx is still a challenging task. The sulfation of active metal oxides and deposition of ammonium bisulfate deactivate catalysts, due to the difficult decomposition of the as-formed sulfate species at low temperatures (<300 °C). In recent years, metal sulfate catalysts have attracted increasing attention owing to their good catalytic activity and strong SO2 tolerance at higher temperatures (>300°C); however, the SO2-tolerant mechanism of metal sulfate catalysts is still ambiguous. In this study, Fe2(SO4)3/TiO2 and Ce2(SO4)3/TiO2 catalysts were prepared using the corresponding metal sulfate salt as the precursor. These catalysts were tested for their low-temperature activity and SO2 tolerance activity. Compared to Ce2(SO4)3/TiO2, Fe2(SO4)3/TiO2 showed significantly better low-temperature activity and SO2 tolerance. It was demonstrated that less surface sulfate species formed on Fe2(SO4)3/TiO2 and Ce2(SO4)3/TiO2. However, the presence of NO and O2 could assist the decomposition of NH4HSO4 over Fe2(SO4)3/TiO2 at a lower temperature, endowing Fe2(SO4)3/TiO2 with better low-temperature SO2 tolerance than Ce2(SO4)3/TiO2. This study unraveled the SO2-tolerant mechanism of Fe2(SO4)3/TiO2 at lower temperatures (<300 °C), and a potential strategy is proposed for improving the low-temperature SO2-tolerance of catalysts with Fe2(SO4)3 as the main active component or functional promoter.

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.

Selective catalytic reduction (SCR) is the most efficient NOX removal technology, and the vanadium-based catalyst is mainly used in SCR technology. The vanadium-based catalyst showed higher NOX removal performance in the high-temperature range but catalytic efficiency decreased at lower temperatures, following exposure to SOX because of the generation of ammonium sulfate on the catalyst surface. To overcome these limitations, we coated an NH4+ layer on a vanadium-based catalyst. After silane coating the V2O5-WO3/TiO2 catalyst by vapor evaporation, the silanized catalyst was heat treated under NH3 gas. By decomposing the silane on the surface, an NH4+ layer was formed on the catalyst surface through a substitution reaction. We observed high NOX removal efficiency over a wide temperature range by coating an NH4+ layer on a vanadium-based catalyst. This layer shows high proton conductivity, which leads to the reduction of vanadium oxides and tungsten oxide; additionally, the NOX removal performance was improved over a wide temperature range. These findings provide a new mothed to develop SCR catalyst with high efficiency at a wide temperature range.

There are still many unsolved mysteries in the thermal decomposition process of urea. This paper studied the thermal decomposition process of urea at constant temperatures by the thermal gravimetric-mass spectrometry analysis method. The results show that there are three obvious stages of mass loss during the thermal decomposition process of urea, which is closely related to the temperature. When the temperature was below 160 °C, urea decomposition almost did not occur, and molten urea evaporated slowly. When the temperature was between 180 and 200 °C, the content of biuret, one of the by-products in the thermal decomposition of urea, reached a maximum. When the temperature was higher than 200 °C, the first stage of mass loss was completed quickly, and urea and biuret rapidly broke down. When the temperature was about 240 °C, there were rarely urea and biuret in residual substance; however, the content of cyanuric acid was still rising. When the temperature was higher than 280°C, there was a second stage of mass loss. In the second stage of mass loss, when the temperature was higher than 330 °C, mass decreased rapidly, which was mainly due to the decomposition of cyanuric acid. When the temperature was higher than 380 °C, the third stage of mass loss occurred. However, when the temperature was higher than 400 °C, and after continuous heating was applied for a sufficiently long time, the residual mass was reduced to almost zero eventually.

The improvement of stability is a crucial and challenging issue for industrial catalyst, which affects not only the service time but also the cost of catalyst. This is especially prominent for that applied in harsh environment atmospheres, such as the exhaust of diesel vehicles. Herein, we reported a new strategy to improve the high-temperature hydrothermal stability of Cu-SSZ-13, which is a promising catalyst for the treatment of exhaust emitted from diesel vehicles through the NH3-SCR NOx route. Different from that reported in literature, we managed to improve the high-temperature hydrothermal stability of Cu-SSZ-13 by coating the surface with a nanolayer of stable SiO2 material using the atomic layer deposition (ALD) method. The coating of SiO2 layers effectively suppressed the leaching of alumina from the SSZ-13 molecular sieve even after the hydrothermal aging at 800 °C for 16 h with 12.5% water in air. Meanwhile, the ultra-thin SiO2 nanolayer does not block the pores of zeolites and affect the catalytic activity of Cu-SSZ-13 contribute to the superiority of the ALD technology.