Activity, stability, and deactivation behavior of supported Au/TiO2 catalysts in the CO oxidation and preferential CO oxidation reaction at elevated temperatures
文摘
The influence of elevated reaction temperatures on the activity, long-time stability, and deactivation behavior of Au/TiO2 catalysts for CO oxidation was studied by kinetic and in situ IR measurements in the temperature range 80–180 °C, both in an idealized, H2-free reaction atmosphere and in a H2-rich gas mixture. The results are discussed in a molecular picture. Most important for practical applications (PROX reaction), the selectivity for CO oxidation in H2-rich gas mixtures decreases sharply with increasing temperature, from 60 % at 80 °C to 15 % at 180 °C. The increasing tendency for H2 oxidation is reflected also by a distinctly lower apparent activation energy for CO oxidation in the presence of H2 (18 ± 3 kJ mol−1) compared to reaction in a H2-free reaction mixture (30 ± 3 kJ mol−1). In all cases, carbonate formation is observed and proposed to contribute to the deactivation, but with different extents depending on the reaction conditions.