From Experiment-Driven to Theory- and Data-Driven: A Computational Paradigm Shift in High-Entropy Electrocatalyst Design.

Abstract

High-entropy materials (HEMs) have emerged as promising electrocatalyst platforms because compositional diversity enables tunable electronic structures and abundant active sites. With rising demands in energy conversion and environmental applications, theory now plays a central role in HEM design, in particular density functional theory (DFT), molecular dynamics (MD), and machine learning (ML). Recent advances in computational strategies for elucidating mechanisms and selecting optimal compositions are synthesized. The shift from experiment-driven studies to proactive, theory- and data-driven discovery is highlighted, enabled by the integration of high-throughput calculations with ML for efficient screening. Method limits and key challenges are assessed, including black-box interpretability, modeling of disorder and coverage, and gaps between theoretical models and experimental conditions, and directions in workflow standardization, open databases, and reproducible benchmarks are outlined. Building on these elements, a compact DFT-ML-MD closed-loop framework is proposed that links atomic-scale energetics to device-level metrics, with the aim of guiding the accelerated discovery and deployment of high-activity, durable high-entropy electrocatalysts for sustainable energy.