Pd catalysts supported on silicon nitride for the combustion of methane: Influence of the crystalline and amorphous phases of the support and of the preparation method on the catalytic performances

Non-oxide refractory materials, such as silicon nitride having high thermal stability and thermal conductivity can be used as catalytic supports. The influence of the Si3N4 support nature and of the chemical compounds used for preparations on the physical-chemistry and catalytic properties of the palladium systems in the total oxidation of methane was investigated. A strong influence of the phase composition and the crystalline state of supports on the catalytic properties in the total oxidation of methane of the Pd catalysts was found. The activity of Pd catalysts increases with the α-Si3N4 content and crystallization state of the support. The catalytic activity of Pd/α-Si3N4 is also strongly affected by the preparation procedure. The Pd/α-Si3N4 catalyst obtained by aqueous impregnation is less active and less stable. It was proposed that if water is used as an impregnation solvent, the surface acid-based properties of Si3N4 support and/or of the Pd active phase are irreversibly damaged. Pd supported on α-Si3N4, prepared by impregnation of the Pd precursors in toluene solutions are found to be the most active and stable under reaction conditions.