Identifying Key Descriptors for the Single-Atom Catalyzed CO Oxidation

Fundamental knowledge of structure-activity correlations for heterogeneous single-atom catalysts (SACs) is essential in guiding catalytic design. While linear scaling relations are powerful for predicting the performance of traditional metal catalysts, they appear to fail with the involvement of SACs. Comparing the catalytic CO oxidation activity of different atomically dispersed metals (3d, 4d, and 5d) in conjunction with computational modeling enabled us to establish multiple scaling relations between the activity and simply calculated descriptors. Through these efforts, we found that the thermodynamic driving force for the oxygen vacancy formation needed to be considered in addition to the adsorption energies of substrates (in particular CO). Our approach was to reduce the computational requirements in determining better CO oxidation catalysts using a few key thermodynamic descriptors. This work presents one of the first successful approaches for re-establishing scaling relations for catalytic reactions by SACs with potentially broad implications for catalytic processes actively involving this support. [GRAPHICS] .

Automated summary

Understanding the structure-activity correlations for heterogeneous single-atom catalysts (SACs) is crucial for catalytic design. In this study, we found that linear scaling relations were not applicable for SACs and established multiple scaling relations between activity and calculated descriptors. The thermodynamic driving force for oxygen vacancy formation was identified as an important factor in addition to substrate adsorption energies, particularly for CO. This work presents a successful approach for re-establishing scaling relations for SACs and has broad implications for catalytic processes involving this type of catalyst.