Catlas: an automated framework for catalyst discovery demonstrated for direct syngas conversion

TL;DR

The paper introduces catlas, an open-source ML framework that automates catalyst discovery by efficiently predicting adsorption energies, demonstrated through identifying promising catalysts for syngas conversion to oxygenates with high accuracy.

Contribution

The paper presents a novel, scalable ML-based framework for catalyst screening that reduces computational costs and enables rapid exploration of large material spaces.

Findings

Predicted adsorption energies with near-DFT accuracy (0.16, 0.14 eV MAE).

Identified 144 promising catalyst candidates for syngas conversion.

Top candidates include unexplored Pt-Ti, Pd-V, Ni-Nb, and Ti-Zn alloys.

Abstract

Catalyst discovery is paramount to support access to energy and key chemical feedstocks in a post fossil fuel era. Exhaustive computational searches of large material design spaces using ab-initio methods like density functional theory (DFT) are infeasible. We seek to explore large design spaces at relatively low computational cost by leveraging large, generalized, graph-based machine learning (ML) models, which are pretrained and therefore require no upfront data collection or training. We present catlas, a framework that distributes and automates the generation of adsorbate-surface configurations and ML inference of DFT energies to achieve this goal. Catlas is open source, making ML assisted catalyst screenings easy and available to all. To demonstrate its efficacy, we use catlas to explore catalyst candidates for the direct conversion of syngas to multi-carbon oxygenates. For this case study, we explore 947 stable/ metastable binary, transition metal intermetallics as possible catalyst candidates. On this subset of materials, we are able to predict the adsorption energy of key descriptors, *CO and *OH, with near-DFT accuracy (0.16, 0.14 eV MAE, respectively). Using the projected selectivity towards C2+ oxygenates from an existing microkinetic model, we identified 144 candidate materials. For 10 promising candidates, DFT calculations reveal a good correlation with our assessment using ML. Among the top elemental combinations were Pt-Ti, Pd-V, Ni-Nb, and Ti-Zn, all of which appear unexplored experimentally.