Interpretable machine learned predictions of adsorption energies at the metal--oxide interface (2505.21428v1)

Abstract: The conversion of $\mathrm{CO_2}$ to value-added compounds is an important part of the effort to store and reuse atmospheric $\mathrm{CO_2}$ emissions. Here we focus on $\mathrm{CO_2}$ hydrogenation over so-called inverse catalysts: transition metal oxide clusters supported on metal surfaces. The conventional approach for computational screening of such candidate catalyst materials involves a reliance on density functional theory (DFT) to obtain accurate adsorption energies at a significant computational cost. Here we present a ML-accelerated workflow for obtaining adsorption energies at the metal--oxide interface. We enumerate possible binding sites at the clusters and use DFT to sample a subset of these with diverse local adsorbate environments. The data set is used to explore interpretable and black-box ML models with the aim to reveal the electronic and structural factors controlling adsorption at metal--oxide interfaces. Furthermore, the explored ML models can be used for low-cost prediction of adsorption energies on structures outside of the original training data set. The workflow presented here, along with the insights into trends in adsorption energies at metal--oxide interfaces, will be useful for identifying active sites, predicting parameters required for microkinetic modeling of reactions on complex catalyst materials, and accelerating data-driven catalyst design.