Abstract
New convenient wet chemistry synthetic routes have made it possible to explore catalytic activities of a variety of single supported atoms. The majority of single supported atoms have been synthesized on active supports which participate in oxidation reactions. The single supported atoms on inert substrates (e.g. alumina) are limited to Pt adatoms and Pd cations, and are generally active toward CO oxidation. In this manuscript, we show that single Pd atoms on θ-alumina show high CO oxidation activity; however, they exhibit no detectable NO oxidation under our experimental conditions. This led us to employ first principles modeling to explore multiple Langmuir-Hinshelwood-type pathways to explain high CO oxidation activity but lack of NO oxidation activity. For completeness, we have also examined Eley-Riedel pathways. We find that a pathway that involves carbonate or nitrate as an intermediate can explain the experimental results of CO and NO oxidation on single alumina supported Pd cations.
