Novel in-situ reduction approach was applied for the synthesis of palladium nanoparticles in the pores of mesoporous silica materials with grafted siliconhydride groups. Matrices possessing different structural proper...Novel in-situ reduction approach was applied for the synthesis of palladium nanoparticles in the pores of mesoporous silica materials with grafted siliconhydride groups. Matrices possessing different structural properties (MCM-41, SBA-15 and Silochrom) were used. Samples were studied by nitrogen adsorption-desorption method, low-angle X-ray diffraction, transmission electron microscopy (TEM) and FT-IR/PAS spectroscopy. The temperature-programmed oxidation (TPO) and reduction (TPR) methods were applied to examine reducibility of palladium species. Palladium containing catalysts were tested in methane oxidation reaction. It was demonstrated that relatively large pores in SBA-15 type silica facilitated formation of well-dispersed palladium nanoparticles confined in the pores channels. In the case of MCM-41 support, metallic palladium nanoparticles were formed on the external surface. The obtained materials showed high catalytic activity. Lower activity of the samples containing small crystallites located in the pore volume at high temperatures was related to worse accessibility of active sites to the reation mixture.展开更多
基金This work was supported by European Community,seventh Framework Programm(FP/2007-2013)Marie Curie International Research Staff Exchange Scheme(grant no.230790)project MEC 06 MAT2006 01997.
文摘Novel in-situ reduction approach was applied for the synthesis of palladium nanoparticles in the pores of mesoporous silica materials with grafted siliconhydride groups. Matrices possessing different structural properties (MCM-41, SBA-15 and Silochrom) were used. Samples were studied by nitrogen adsorption-desorption method, low-angle X-ray diffraction, transmission electron microscopy (TEM) and FT-IR/PAS spectroscopy. The temperature-programmed oxidation (TPO) and reduction (TPR) methods were applied to examine reducibility of palladium species. Palladium containing catalysts were tested in methane oxidation reaction. It was demonstrated that relatively large pores in SBA-15 type silica facilitated formation of well-dispersed palladium nanoparticles confined in the pores channels. In the case of MCM-41 support, metallic palladium nanoparticles were formed on the external surface. The obtained materials showed high catalytic activity. Lower activity of the samples containing small crystallites located in the pore volume at high temperatures was related to worse accessibility of active sites to the reation mixture.
