Bio-Inspired Hierarchical Nanoreactor With Hetero-Coordinated Fe-P-Co Bridges for Whole-Pathway-Regulated Electrocatalytic Oxygen Reduction
[EN] Efficient oxygen reduction reaction (ORR) requires coordination of oxygen adsorption, transport, and catalysis at active sites. Yet most studies address only one step, overlooking whole-pathway O2 regulation and thus limiting performance. Here, we report a bioinspired Co-doped Fe2P on N-doped c...
| Autores: | , , , , , , , |
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| 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:dnet:riunet______::e40019d462ed20cf99244c6955067dd6 |
| Acceso en línea: | https://riunet.upv.es/handle/10251/233499 |
| Access Level: | acceso abierto |
| Palabra clave: | Co-Fe electronic synergy ORR performance Eucalyptus-like nanotube Hetero-coordinated Fe P Co bridges Oxygen adsorption and transport dynamics |
| Sumario: | [EN] Efficient oxygen reduction reaction (ORR) requires coordination of oxygen adsorption, transport, and catalysis at active sites. Yet most studies address only one step, overlooking whole-pathway O2 regulation and thus limiting performance. Here, we report a bioinspired Co-doped Fe2P on N-doped carbon featuring a hierarchical eucalyptus-like nanoarchitecture, engineered to regulate oxygen throughout the electrochemical cycle, where Fe-P-Co hetero-coordinated bridges anchored to the carbon substrate through Fe & horbar;N bonds induce strong electronic coupling and polarization. The hierarchical structure generated local electric fields that enriched OH- and O2, while multilevel porosity accelerated oxygen transport. This enabled coordinated optimization of oxygen adsorption, transfer, and active-site electronic configuration. This nanohybrid achieved a half-wave potential of 0.938 V vs. RHE, sustained discharge in Al-air batteries for 373 h, and delivered an energy density of 3487 Wh/kg. Theoretical simulations revealed that Co-doping shortened Fe & horbar;P bonds and tuned the Fe electronic environment, lowering the d-band center and weakening Fe 3d-O 2p interactions, which reduced the *OH desorption barrier and accelerated ORR kinetics. In situ Raman spectroscopy revealed that Fe-P-Co bridges served as active centers facilitating *OH release during ORR. These findings indicate that integrating hierarchical architecture, hetero-coordinated Fe-P-Co bridges, and electronic-state modulation enables whole-pathway O2 management for efficient oxygen electrocatalysis. |
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