Theoretical Insights into 4f–3d Synergistic Catalysis in Fe–Light Rare-Earth Atomic-Scale Catalysts for Oxygen Reduction

Résumé fourni par la source

Sluggish oxygen reduction reaction (ORR) kinetics limit energy conversion efficiency, driving research interest in atomic-level catalysts. This work employs density functional theory calculations to investigate the ORR activity of Fe-based light rare-earth catalysts. Six Fe-light rare-earth configurations are constructed to reveal how 4f orbitals modulate the electronic structure of the Fe sites. Gibbs free energy analyses reveal synergistic catalysis between Fe and light rare-earth elements, enabling catalysts to optimize the reaction pathway and lower energy barriers of intermediates compared to single-atom catalysts. Among these, Fe-Nd-NC exhibits an ORR performance with an overpotential of only 0.55 V, an improvement over Fe-N-C and Nd-N-C. Electronic state analyses identify Fe atoms as active sites and Nd atoms as modulation centers. The 4f-3d coupling yields an optimal structure, optimizing the configuration of Fe sites and tuning the adsorption strength of intermediates. This study elucidates the origin of synergistic catalysis in Fe-light rare-earth catalysts, offering theoretical guidance for the design of ORR electrocatalysts.

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