ABSTRACT 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 O 2 regulation and thus limiting performance. Here, we report a bioinspired Co‐doped Fe 2 P 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─N bonds induce strong electronic coupling and polarization. The hierarchical structure generated local electric fields that enriched OH − and O 2 , 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─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 O 2 management for efficient oxygen electrocatalysis.
Xu et al. (Sun,) studied this question.
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