Single-atom Ir₁ supported on rutile TiO₂ for excellent selective catalytic oxidation of ammonia

Gaseous ammonia (NH₃) in the atmosphere is potentially harmful to both human health and the environment. The selective catalytic oxidation of NH₃ (termed as NH₃-SCO) into N₂ and H₂O is a promising method for decreasing NH₃ emissions. A highly efficient catalyst is required for controlling NH₃ emissions by this method in practice. In this study, we prepared Ir/TiO₂ catalysts using different crystal structures of TiO₂ (rutile, P25 or anatase) as supports by a simple impregnation method and evaluated their performance in the NH₃-SCO. We found that the Ir/TiO₂-R (rutile) catalyst performed better than the Ir/TiO₂-P25 (mixed-phase) and Ir/TiO₂-A (anatase) catalyst. High-angle annular dark-field images of the aberration-corrected scanning transmission electron microscopy revealed that the Ir species were mainly atomically dispersed on the TiO₂ support in Ir/TiO₂-R with 1 wt% Ir loading, whereas the Ir species agglomerated to form clusters or nanoparticles in Ir/TiO₂-P25 and Ir/TiO₂-A. The combined results of X-ray absorption fine structure, H₂-temperature-programmed reduction, and in situ diffuse reflectance for infrared Fourier Transform spectroscopy studies suggested that atomically dispersed Ir species had stronger electronic metal-support interaction with rutile TiO₂, which resulted in easier to adsorb and activate O₂ at the interface and thus, better low-temperature activity of the Ir/TiO₂-R catalyst.