Compositional Phase Control in High-Entropy Alloy Electrocatalysts

Jeong, Sangmin; Branco, Anthony J.; Nagarajan, Porvajja; Sullivan, Connor S.; Cha, Ji Hyeon; Bollen, Silas W.; Mason, Noah L.; Abeykoon, Milinda; Olds, Daniel; Ross, Michael B.

doi:10.1021/jacs.5c16422

Title: Compositional Phase Control in High-Entropy Alloy Electrocatalysts

Journal Article · Thu Jan 22 00:00:00 UTC 2026 · Journal of the American Chemical Society

DOI: https://doi.org/10.1021/jacs.5c16422 · OSTI ID:3017938

^[1]; Branco, Anthony J. ^[1]; Nagarajan, Porvajja ^[1]; Sullivan, Connor S. ^[1]; Cha, Ji Hyeon ^[1]; Bollen, Silas W. ^[1]; Mason, Noah L. ^[1]; Abeykoon, Milinda ^[2]; Olds, Daniel ^[2];

^[1]

Univ. of Massachusetts, Lowell, MA (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

High-entropy alloys (HEAs) provide uniquely tunable structural and electronic properties that enable robust electrocatalysis. While compositional manipulation of HEAs is well-known, systematically controlling the crystalline phase and morphology remains a challenge that could provide new avenues for controlling reactive sites and physical properties. Here, we show the preferential stabilization of mixed fcc/bcc to fcc phases by controlling the Au content in quinary AuPdFeCoNi HEA nanoparticles. This systematic structural and compositional control, when investigated with an ensemble of electronic, X-ray synchrotron, and surface techniques, allows us to identify the critical short- (few-Å) and medium- (6–10 Å) range structural motifs that deliver exceptional hydrogen evolution reaction (HER) catalysis. Specifically, these HEAs exhibit both outstanding durability (240 h) and high mass activity (50 A/mg_PGM) normalized to noble metal content, outperforming commercial Pt/C (3.18 A/mg_PGM). This structural control over HEA morphology, and its direct association with changes in specific metallic oxidation states and pair–pair atomic structural features, provides new means and strategies for finely designing robust and sustainable electrocatalysts with a majority nonprecious metal composition.

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Research Organization:: Brookhaven National Lab; Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: Brookhaven National Lab; Office of Naval Research; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: SC0012704

OSTI ID:: 3017938

Report Number(s):: BNL-229403-2026-JAAM

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 5 Vol. 148; ISSN 0002-7863; ISSN 1520-5126

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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alloys
electrocatalysts
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gold
nanoparticles

Title: Compositional Phase Control in High-Entropy Alloy Electrocatalysts

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