Uncovering Stability Origins in Layered Ferromagnetic Electrocatalysts Through Homolog Comparison

Uncovering Stability Origins in Layered Ferromagnetic Electrocatalysts Through Homolog Comparison

Magnetic 2D materials offer a compelling platform for next-generation electrocatalysis by enabling spin-dependent reaction pathways. Among them, layered ferromagnets such as Fe<sub>3</sub>GeTe<sub>2</sub> (FGT) have garnered attention for combining intrinsic ferromagnetism wi...

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Main Authors: Om Prakash Gujela, Sivasakthi Kuppusamy, Yu-Xiang Chen, Chang-Chi Kao, Jian-Jhang Lee, Bhartendu Papnai, Ya-Ping Hsieh, Raman Sankar, Mario Hofmann
Format: Article
Language:English
Published: MDPI AG 2025-08-01
Series:Nanomaterials
Subjects:
electrocatalysis
hydrogen evolution reaction
single-crystal growth
ferromagnetic layered materials
cyclic voltammetry
Online Access:https://www.mdpi.com/2079-4991/15/15/1210
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Summary:Magnetic 2D materials offer a compelling platform for next-generation electrocatalysis by enabling spin-dependent reaction pathways. Among them, layered ferromagnets such as Fe<sub>3</sub>GeTe<sub>2</sub> (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 Fe<sub>3</sub>GaTe<sub>2</sub> (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.
ISSN:2079-4991

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