High-Temperature Behavior of Pd/MgO Catalysts Prepared via Various Sol–Gel Approaches

Abstract

A series of Pd/MgO catalysts based on nanocrystalline MgO were prepared via different sol–gel approaches. In the first two cases, palladium was introduced during the gel preparation, followed by drying it in supercritical or ambient conditions. In the third case, aerogel-prepared MgO was impregnated with an ethanol solution of Pd(NO3)2. The prepared catalysts differ in particle size and oxidation state of palladium. The catalytic performance and thermal stability of the samples were examined in a model reaction of CO oxidation at prompt thermal aging conditions. The as-prepared and aged materials were characterized by low-temperature nitrogen adsorption, UV-vis spectroscopy, X-ray photoelectron spectroscopy, transmission electron microscopy, and ethane hydrogenolysis testing reaction. The highest initial activity (T50 = 103 °C) was demonstrated by the impregnated sample, containing Pd0 particles of 3 nm in size. The lowest T50 value (215 °C) after aging at 1000 °C was demonstrated by the impregnated Pd/MgO-WI sample. The high-temperature behavior of the catalysts was found to be affected by the initial oxidation state and dispersion of Pd. Two deactivation mechanisms, such as the agglomeration of Pd particles and migration of small Pd species into the bulk of the MgO support with the formation of Pd-MgO solid solutions, were discussed.

Keywords

• magnesium oxide
• sol–gel synthesis
• palladium catalysts
• CO oxidation
• prompt thermal aging
• metal–support interactions