Asymmetric Enhancement of Hydrogen and Oxygen Evolution Reactions in a Bifunctional Fe0.5Rh0.5 Catalyst by Applying a
Hang Xu1, Linglong Hu1, Ji Qi2
1Key Laboratory of Functional Materials Physics and Chemistry of the Ministry of Education, Jilin Normal University, Changchun 130103, China.
Abstract:
Magnetic field enhancement represents an effective strategy to promote electrocatalytic water splitting, yet the mechanistic origin of asymmetric hydrogen evolution reaction (HER)/oxygen evolution reaction (OER) promotion remains poorly understood. Here, we investigate a bifunctional Fe0.5Rh0.5 (FeRh) single-crystal thin-film catalyst and demonstrate distinct asymmetric activity improvement under a 13 kOe magnetic field, ∼40% enhancement for HER and ∼32% for OER. Density functional theory and spin-resolved electronic structure analysis reveal that the field raises spin polarization by 1.2%, enhances density of states near the Fermi level, and accelerates interfacial charge transfer. The asymmetric enhancement stems from a more significant Gibbs free energy reduction for H adsorption than for OH**. Moreover, FeRh follows the oxide pathway mechanism to avoid excessive surface oxyhydroxide passivation, ensuring a stable magneto-responsive catalysis. This work clarifies the fundamental mechanism of asymmetric magnetic field promotion and provides a rational design for magnetically enhanced bifunctional electrocatalysts.
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