Uncovering Stability Origins in Layered Ferromagnetic Electrocatalysts Through Homolog Comparison

TL;DR

This study explores why some magnetic materials degrade in electrochemical reactions and how to design more stable ones.

Contribution

The paper introduces a structural homolog approach to separate catalytic activity from degradation in magnetic electrocatalysts.

Findings

FGT's electrochemical activity is mainly due to Fe orbitals and is insensitive to sublayer composition.

FGaT shows lower long-term stability due to weaker Te bonding from Ga substitution.

Structural homologs help decouple activity from degradation in magnetic electrocatalysts.

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.

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