Investigation into the impact of CeO2 morphology regulation on the oxidation process of dichloromethane.

Four distinct CeO2 catalysts featuring varied morphologies (nanorods, nanocubes, nanoparticles, and nano spindle-shaped) were synthesized through a hydrothermal process and subsequently employed in the oxidation of dichloromethane (DCM). The findings revealed that the nano spindle-shaped CeO2 exhibited exposure of crystal faces (111), demonstrating superior catalytic oxidation performance for DCM with a T90 of 337 °C and notably excellent low-temperature catalytic activity (T50 = 192 °C). The primary reaction products were identified as HCl and CO2. Through obvious characterizations, it showed that the excellent catalytic activity presented by CeO2-s catalyst might be related to the higher oxygen vacancy concentration, surface active oxygen content, and superior redox performance caused by specific exposed crystal planes. Meanwhile, CeO2-s catalyst owned outstanding stability, reusability, and water inactivation regeneration, which had tremendous potential in practical treatment.

Insights into the superior resistance of In-Co3O4-Ga2O3/H-Beta to SO2 and H2O in the selective catalytic reduction of NOx by CH4.

The existence of sulfur dioxide and water vapor in the flue gas generated from waste-to-energy stations could lead to catalyst deactivation, which has adverse effects on NOx removal. It is thus particularly important to study the reaction mechanism of catalyst resistance to poisoning. Herein, we report the mechanism of In-Co3O4-Ga2O3/H-Beta catalyst to SO2 and H2O resistance in the selective catalytic reduction (SCR) of NOx by CH4. The catalyst could achieve 74.6% NOx removal efficiency in the presence of 100 ppm SO2 and 5% H2O. In this catalyst, Co3O4 is attributed to enhancing the reversible poisoning of SO2 and CH4 activation and increasing the number of Brønsted acid sites by decomposing H2O. However, the InO+ active center was still eroded by a small amount of water vapor, leading to a reduction in NOx removal efficiency. The addition of Ga2O3 primarily provided an important intermediate NO2 for CH4-SCR reaction and reduced the aggregates of Co3O4 to increase the exposure of indium sites, and could reduce a part of SO2 to S2-. This study provides a good candidate for preparing catalysts with superior resistance towards SO2 and H2O for CH4-SCR.

Amino-acid modulated hierarchical In/H-Beta zeolites for selective catalytic reduction of NO with CH4 in the presence of H2O and SO2.

Selective catalytic reduction of NO with CH4 (CH4-SCR) has been studied over a series of amino-acid mediated hierarchical beta zeolites with indium exchange. Amino acid mesoporogens greatly affect the NO reduction (DeNOx) efficiency of In/H-Beta catalysts. Mesoporous In/H-Beta-P synthesized using proline exhibits the highest NOx removal efficiency of 40% in excess oxygen and poisonous SO2 and H2O, 10% higher than our previously optimized In/H-Beta catalyst using commercial beta zeolites with a similar Si/Al ratio. Analyses using XRD, N2 adsorption-desorption, EPR, SEM, TEM, EDX, ICP, 27Al and 29Si MAS NMR, XPS, H2-TPR, NH3-TPD, and Py-IR reveal that amino acids promote beta crystallization, modulate zeolite acid sites and surface oxygen species, and generate hierarchical pore architectures without affecting the Si/Al ratio, indium content, and percentage of the active InO+ species. The mosaic-structured In/H-Beta-P exhibits the strongest Brønsted acidity and surface labile oxygen which enhance the oxyindium interaction with the zeolite framework, promoting CH4-SCR activity. The strong acidity, surface active oxygen species, and mesopores lead to excellent stability of the In/H-Beta-P catalyst in the presence of SO2 and H2O, withstanding several catalytic DeNOx cycles under harsh reaction conditions.

Effect of preparation and reaction conditions on the performance of In/H-Beta for selective catalytic reduction of NOx with CH4.

In/H-Beta catalyst was prepared by optimizing the support, concentration of ion exchange liquid and calcination temperature to investigate the effects of synthesis conditions on catalytic activity of selective catalytic reduction of NOx with CH4. The results showed that the In/H-Beta catalyst exhibited the superior activity when concentration of exchange liquid was 0.033 M and calcination temperature was 500 °C, the NOx removal ratio could reach 97.6%. In addition, reaction conditions could affect the catalytic performance. When O2 concentration was 10%, CH4:NO ratio was no less than one, space velocity was lower than 23600 h-1 and NO initial concentration was no more than 700 ppm, In/H-Beta could exhibit superior catalytic activity. Moreover, the catalytic performances of In/H-Beta catalysts were discussed after enduring H2O or/and SO2. This novel strategy could open the door for selective catalytic reduction of NOx with CH4.