Uncovering Stability Origins in Layered Ferromagnetic Electrocatalysts Through Homolog Comparison
Journal
Nanomaterials
Journal Volume
15
Journal Issue
15
Start Page
1210
ISSN
2079-4991
Date Issued
2025-08-07
Author(s)
Gujela, Om Prakash
Kuppusamy, Sivasakthi
Chen, Yu-Xiang
Kao, Chang-Chi
Lee, Jian-Jhang
Papnai, Bhartendu
Hsieh, Ya-Ping
Sankar, Raman
Abstract
Magnetic 2D materials offer a compelling platform for next-generation electrocatalysis by enabling spin-dependent reaction pathways. Among them, layered ferromagnets such as Fe3GeTe2 (FGT) have garnered attention for combining intrinsic ferromagnetism with high predicted oxygen evolution activity. However, the stability of non-oxide ferromagnets in electrochemical environments remains an unresolved challenge, limiting their envisioned applications. In this study, we introduce a structural homolog approach to investigate the origin of FGT’s catalytic behavior and the mechanisms underlying its degradation. By comparing FGT with its isostructural analog Fe3GaTe2 (FGaT), we demonstrate that the electrochemical activity of FGT arises primarily from Fe orbitals and is largely insensitive to changes in sublayer composition. Although both materials exhibit similar basal-plane hydrogen evolution performance, FGaT demonstrates significantly lower long-term stability. Density functional theory calculations reveal that this instability arises from weaker Te bonding introduced by Ga substitution. These findings establish structural homologs as a powerful strategy for decoupling catalytic activity from electrochemical deterioration and for guiding the rational design of stable magnetic electrocatalysts.
Subjects
cyclic voltammetry
electrocatalysis
ferromagnetic layered materials
hydrogen evolution reaction
single-crystal growth
Publisher
MDPI AG
Type
journal article