Interfacial electron flow in a Fe2P@NPC(core)/NiCo LDH(shell) heterostructure enables site-specific electronic-state modulation for bifunctional oxygen electrocatalysis

[EN] Efficient bifunctional electrocatalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are vital for next-generation rechargeable Zn-air batteries (ZABs). Yet, achieving robust interfacial coupling and precise electronic state matching between ORR and OER sites remains...

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Detalles Bibliográficos
Autores: Xu, Qiaoling, Zhang, Lei, Liu, Changlang, Zhao, Xue, Zhang, Yongcai, Zhou, Yingtang, García Gómez, Hermenegildo|||0000-0002-9664-493X
Tipo de recurso: artículo
Fecha de publicación:2026
País:España
Institución:Universitat Politècnica de València (UPV)
Repositorio:RiuNet. Repositorio Institucional de la Universitat Politécnica de Valéncia
Idioma:inglés
OAI Identifier:oai:riunet.upv.es:10251/233174
Acceso en línea:https://riunet.upv.es/handle/10251/233174
Access Level:acceso embargado
Palabra clave:Active site assembly
Multiple-bridged interface
Electron density distribution
Oxygen reduction
Oxygen evolution
Descripción
Sumario:[EN] Efficient bifunctional electrocatalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are vital for next-generation rechargeable Zn-air batteries (ZABs). Yet, achieving robust interfacial coupling and precise electronic state matching between ORR and OER sites remains challenging. Here, we devised a proof-ofconcept strategy based on a multiple-bridged interface that induced directed electron flow between ORR-active Fe2P@N/P-doped carbon (NPC) and OER-active NiCo-layered double hydroxides (LDH). This configuration bridged Fe2P to the NPC substrate via Fe-N bonds and formed a semi-coherent interface with LDH, resulting in a bifunctional catalyst with an exceptionally low Delta E of 0.581 V. When integrated into ZABs, the catalyst delivered a peak power density of 220 mW/cm2, a specific capacity of 792 mAh/gZn, and decent cycling stability. In-situ measurements and theoretical analyses revealed charge transfer from LDH through Fe2P to NPC across the interface, enabling site-specific electronic-state modulation. This generated an electron-deficient LDH favorable for OER while optimizing the electronic state of Fe2P for enhanced ORR activity. This facilitated rapid *O to *OOH conversion at LDH sites during OER and promoted *OH desorption at Fe2P sites during ORR. Therefore, our work shows that adequate interfacial charge transfer enables site-specific electronic state control for synergistic oxygen electrocatalysis.