Unraveling Reactivity Origin of Oxygen Reduction at High-Entropy Alloy Electrocatalysts with a Computational and Data-Driven Approach.

High-entropy alloys (HEAs), characterized as compositionally complex solid solutions with five or more metal elements, have emerged as a novel class of catalytic materials with unique attributes. Because of the remarkable diversity of multielement sites or site ensembles stabilized by configurational entropy, human exploration of the multidimensional design space of HEAs presents a formidable challenge, necessitating an efficient, computational and data-driven strategy over traditional trial-and-error experimentation or physics-based modeling. Leveraging deep learning interatomic potentials for large-scale molecular simulations and pretrained machine learning models of surface reactivity, our approach effectively rationalizes the enhanced activity of a previously synthesized PdCuPtNiCo HEA nanoparticle system for electrochemical oxygen reduction, as corroborated by experimental observations. We contend that this framework deepens our fundamental understanding of the surface reactivity of high-entropy materials and fosters the accelerated development and synthesis of monodisperse HEA nanoparticles as a versatile material platform for catalyzing sustainable chemical and energy transformations.