(5af) Understanding Transition Metal Catalyzed Oxidations: Toward Catalyst Design

One of the grand challenges in chemical engineering is to find new ways to manipulate chemical phenomena. A prominent application of this goal is controlling the rates of chemical reactions, commonly achieved with catalysts. Catalysts are typically applied on a large scale, but they function at the molecular level. Effective large-scale catalyst design requires an intimate understanding of molecular-level catalytic behavior. Simulation provides a means for understanding, but a dominant challenge is bridging the gap between microscopic models and macroscopic behavior. In this work we show how careful molecular simulation and thermodynamic and kinetic modeling were used in collaboration with experimental observation to elucidate the key features in Pt-catalyzed NO oxidation, an important process in NOx remediation that occurs in strongly oxidizing conditions. The results pave the way for catalyst design and make implications for other catalyzed oxidations. Future work in these areas will be discussed.