Lowering the Operating Temperature of Perovskite Catalysts for N2O Decomposition through Control of Preparation Methods

Abstract

Discovering catalysts that can decompose N2O at low temperatures represents a major challenge in modern catalysis. The effect of preparative route on N2O-decomposition activity has been examined for a PrBaCoO3 perovskite catalyst. Initially, a citric acid preparation was utilised where the A site ratio was altered in order to increase phase purity. Comparable compositions were then prepared by an oxalic acid precipitation method and by a supercritical anti-solvent technique to produce perovskites with a higher surface area (> 30 m2g-1). By altering the A site ratios it was possible to reduce the temperature required to produce a pure phase perovskite whilst maintaining a higher-surface area. The use of the different preparation methods resulted in perovskites with varying properties, as determined by N2 adsorption, XPS and O2-TPD. This work confirms the importance of lattice oxygen species that have high oxygen mobility for enhanced decomposition of N2O, as oxygen recombination is considered the rate-limiting step. Here, the formation of molecular oxygen is limited by surface adsorbed O species being within a distance at which oxygen recombination is possible. The most active PrBaCo-based catalyst did not have the highest percentage of lattice oxygen as shown by XPS, however, the catalytic activity could be correlated to the mobile oxygen species and high surface area. The PrBaCo-based catalyst prepared by supercritical anti-solvent converted 50 % of the N2O present in the feed (T50) at 410 °C, which represents a significant improvement over reported catalytic performance measured under similar conditions.