Alkali/alkaline-earth metal-modified MnOx supported on three-dimensionally ordered macroporous–mesoporous TixSi1-xO2 catalysts: Preparation and catalytic performance for soot combustion

Abstract

The performance of catalysts used in after-treatment systems is the key factor for the removal of diesel soot, which is an important component of atmospheric fine particle emissions. Herein, three-dimensionally ordered macroporous–mesoporous TixSi1-xO2 (3DOM-m TixSi1-xO2) and its supported MnOx catalysts doped with different alkali/alkaline-earth metals (AMnOx/3DOM-m Ti0.7Si0.3O2 (A: Li, Na, K, Ru, Cs, Mg, Ca, Sr, Ba)) were prepared by mesoporous template (P123)-assisted colloidal crystal template (CCT) and incipient wetness impregnation methods, respectively. Physicochemical characterizations of the catalysts were performed using scanning electron microscopy, X-ray diffraction, N2 adsorption–desorption, H2 temperature-programmed reduction, O2 temperature-programmed desorption, NO temperature-programmed oxidation, and Raman spectroscopy techniques; then, we evaluated their catalytic performances for the removal of diesel soot particles. The results show that the 3DOM-m Ti0.7Si0.3O2 supports exhibited a well-defined 3DOM-m nanostructure, and AMnOx nanoparticles with 10–50 nm were evenly dispersed on the inner walls of the uniform macropores. In addition, the as-prepared catalysts exhibited good catalytic performance for soot combustion. Among the prepared catalysts, CsMnOx/3DOM-m Ti0.7Si0.3O2 had the highest catalytic activity for soot combustion, with T10, T50, and T90 (the temperatures corresponding to soot conversion rates of 10%, 50%, and 90%) values of 285, 355, and 393°C, respectively. The high catalytic activity of the CsMnOx/3DOM-m Ti0.7Si0.3O2 catalysts was attributed to their excellent low-temperature reducibility and homogeneous macroporous–mesoporous structure, as well as to the synergistic effects between Cs and Mn species and between CsMnOx and the Ti0.7Si0.3O2 support.