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Updated: Aug 6, 2026
09:18
Simple Methods for the Preparation of Non-noble Metal Bulk-electrodes for Electrocatalytic Applications
Published on: June 21, 2017
Coverage-Dependent Lateral Interactions Shape the Electrocatalytic Activity of High-Entropy Alloys
Pengfei Hou1, Jin-Cheng Liu1,2
1Center for Rare Earth and Inorganic Functional Materials, School of Materials Science and Engineering & National Institute for Advanced Materials, Nankai University, Tianjin300350, China.
Journal of the American Chemical Society
|July 20, 2026
Summary
Machine learning models lateral interactions in high-entropy alloys (HEAs) for oxygen reduction reactions (ORR). This reveals how surface crowding impacts catalyst design, improving predictions for better electrocatalyst development.
Area of Science:
- Materials Science
- Electrochemistry
- Computational Chemistry
Background:
- High-entropy alloys (HEAs) offer diverse surface sites for electrocatalysis.
- Theoretical studies often overlook coverage-dependent lateral interactions crucial for reactive interfaces.
Purpose of the Study:
- To develop a machine learning framework for modeling the oxygen reduction reaction (ORR) in HEAs.
- To investigate the impact of lateral interactions on electrocatalytic activity in complex alloy systems.
Main Methods:
- Utilized a machine learning interatomic potential (MLIP)-enabled framework.
- Modeled the ORR within a broad Ag-Ir-Ru-Pd-Pt-Cu-Rh-Re alloy composition space.
- Tracked binding strengths of O* and OH* intermediates under competitive coadsorption.
Main Results:
- Highlighted the significant role of lateral interactions (hydrogen-bonding, electrostatic repulsion) in determining electrocatalytic activity.
- Demonstrated improved agreement with experimental trends by including coverage effects.
- Showed that increased compositional complexity can amplify lateral repulsion, reducing optimal active sites.
Conclusions:
- Coverage-dependent lateral interactions are critical for accurate theoretical prediction of HEA electrocatalytic activity.
- The interplay between local electronic effects and lateral interactions dictates a volcano-shaped activity-entropy relationship.
- This framework provides guidance for the rational design of novel HEA-based ORR electrocatalysts.
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