Materials Chemistry and Physics, Vol.139, No.1, 125-133, 2013
Cerium incorporating into MCM-41 mesoporous materials for CO oxidation
Ceria doped MCM-41 materials were synthesized by surfactant-assisted hydrothermal and wet impregnation methods. All the obtained Ce-MCM-41 materials were characterized by N-2 physical adsorption, X-ray diffraction (XRD), diffuse reflectance UV-visible spectroscopy (DRUV-vis), infrared spectroscopy (IR), solid-state cross-polarization magic angle spinning nuclear magnetic resonance spectroscopy (CP/MAS-NMR), and transmission electron microscopy (TEM). The catalytic properties were evaluated in CO oxidation under atmospheric pressure and various temperatures. The results showed that in the materials synthesized by hydrothermal method, most of Ce ions were well incorporated in the tetrahedral coordinated sites into the framework of the MCM-41 as Si/Ce molar ratio is 30 and 50. High cerium content may lead to mesostructure partial collapsing and ceria particles segregation. For CO oxidation, the catalytic activity of Ce-MCM-41 synthesized by hydrothermal method was significantly greater than that of the materials prepared by impregnation route. Over the Ce-MCM-41 materials prepared via hydrothermal technique, 100% CO conversion was achieved at 504, 514 and 528 K, respectively, as the Si/Ce molar ratio decreased from 50 to 30 and 10. For the first time, we found an interesting correlation of Q(3) species relative area in the Si-29 CP/MAS-NMR spectra of the Ce-MCM-41 materials with the reaction rates of CO oxidation, which indicates that both surface hydroxyls and tetrahedral-coordinated Ce4+ ions in the MCM-41 take important roles in the CO oxidation. (C) 2013 Elsevier B.V. All rights reserved.
Keywords:Surface properties;Fourier transform infrared spectroscopy (FTIR);Nuclear magnetic Resonance (NMR);Electron microscopy (STEM;TEM and SEM);Oxidation