WhereWulff: A Semiautonomous Workflow for Systematic Catalyst Surface Reactivity under Reaction Conditions.

Abstract

This paper introduces WhereWulff, a semiautonomous workflow for modeling the reactivity of catalyst surfaces. The workflow begins with a bulk optimization task that takes an initial bulk structure and returns the optimized bulk geometry and magnetic state, including stability under reaction conditions. The stable bulk structure is the input to a surface chemistry task that enumerates surfaces up to a user-specified maximum Miller index, computes relaxed surface energies for those surfaces, and then prioritizes those for subsequent adsorption energy calculations based on their contribution to the Wulff construction shape. The workflow handles computational resource constraints such as limited wall-time as well as automated job submission and analysis. We illustrate the workflow for oxygen evolution reaction (OER) intermediates on two double perovskites. WhereWulff nearly halved the number of Density Functional Theory (DFT) calculations from ∼240 to ∼132 by prioritizing terminations, up to a maximum Miller index of 1, based on surface stability. Additionally, it automatically handled the 180 additional resubmission jobs required to successfully converge 120+ atoms systems under a 48-h wall-time cluster constraint. There are four main use cases that we envision for WhereWulff: (1) as a first-principles source of truth to validate and update a closed-loop self-sustaining materials discovery pipeline, (2) as a data generation tool, (3) as an educational tool, allowing users (e.g., experimentalists) unfamiliar with OER modeling to probe materials they might be interested in before doing further in-domain analyses, (4) and finally, as a starting point for users to extend with reactions other than the OER, as part of a collaborative software community.