Predicting binding motifs of complex adsorbates using machine learning with a physics-inspired graph representation

Abstract: Computational screening in heterogeneous catalysis relies increasingly on machine learning models for predicting key input parameters due to the high cost of computing these directly using first-principles methods. This becomes especially relevant when considering complex materials spaces, e.g. alloys, or complex reaction mechanisms with adsorbates that may exhibit bi- or higher-dentate adsorption motifs. Here we present a data-efficient approach to the prediction of binding motifs and associated adsorption enthalpies of complex adsorbates at transition metals (TMs) and their alloys based on a customized Wasserstein Weisfeiler-Lehman graph kernel and Gaussian Process Regression. The model shows good predictive performance, not only for the elemental TMs on which it was trained, but also for an alloy based on these TMs. Furthermore, incorporation of minimal new training data allows for predicting an out-of-domain TM. We believe the model may be useful in active learning approaches, for which we present an ensemble uncertainty estimation approach.