Surface science provides a multitude of methods for interrogating catalyst and the reactions taking place on them at the atomic and molecular levels. Researchers decipher instrumental output to obtain information regarding the state of the catalytic surface and mechanism and energetics of the reaction. Instrumentation represents a complex response function whose output is not invertible, making the interpretation of spectroscopic and imaging results non-trivial that has largely remained experiential. First principles theoretical calculation nicely complements the surface science approach to catalysis by making it possible to simulate the response of multiple types of instrument and efficiently test hypothetical models, while simultaneously offering quantitative energetic information. It has been shown to be a valuable tool to connect fundamental surface science with an applied science that is catalysis by many excellent studies.<br/><br/>In this talk, I will highlight some collaborative efforts that my group has been involved in where theoretical contributions are combined with surface science experiments to elucidate the details of surface reactions on common catalytic materials. We establish the identities of reaction intermediates by achieving agreement between simulations and spectroscopic experiments. In turn, mechanisms are proposed that explicitly take into account such intermediates. Then based on the kinetic and thermodynamic parameters obtained from DFT calculations, we predict surface reactivity e.g., with respect to temperature, which is compared with experimental observations. By doing so the mechanism of a surface reaction can be established with a high degree of confidence. Examples to be discussed will include acetaldehyde on CeO<sub>2</sub>(111) and hydrogen cyanide on Pd(111).

Theory as a bridge between surface science and catalysis

ACS Spring 2022

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