Invariant Molecular Representations for Heterogeneous Catalysis.

Catalyst screening is a critical step in the discovery and development of heterogeneous catalysts, which are vital for a wide range of chemical processes. In recent years, computational catalyst screening, primarily through density functional theory (DFT), has gained significant attention as a method for identifying promising catalysts. However, the computation of adsorption energies for all likely chemical intermediates present in complex surface chemistries is computationally intensive and costly due to the expensive nature of these calculations and the intrinsic idiosyncrasies of the methods or data sets used.

Benchmarking the Accuracy of Density Functional Theory against the Random Phase Approximation for the Ethane Dehydrogenation Network on Pt(111).

The Random Phase Approximation (RPA) is conceptually the most accurate Density Functional Approximation method, able to simultaneously predict both adsorbate and surface energies accurately; however, this work questions its superiority over DFT for catalytic application on hydrocarbon systems. This work uses microkinetic modeling to benchmark the accuracy of DFT functionals against that of RPA for the ethane dehydrogenation reaction on Pt(111). Eight different functionals, with and without dispersion corrections, across the GGA, meta-GGA and hybrid classes are evaluated: PBE, PBE-D3, RPBE, RPBE-D3, BEEF-vdW, SCAN, SCAN-rVV10, and HSE06.