Phosphorus-Doping Drives the Formation of a Pt-Skin@PtFe Alloy Catalyst With Modulated d-Band Center for Oxygen Reduction AITranslate

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Platinum (Pt)-based catalysts are crucial for the commercialization of hydrogen/metal air batteries, but they suffer from Pt scarcity, high cost, and nanoparticle dissolution/agglomeration, mainly leading to performance degradation. We address this by synthesizing a PtFe alloy catalyst (PtFe–PA–NC) via a phytic acid (PA) assisted pyrolysis strategy, featuring Pt-skin-coated PtFe alloy nanoparticles on hierarchically porous N-doped carbon (NC). PA treatment simultaneously enhances the support's surface area and pore structure for better mass transport, and incorporates P into the carbon framework via P–C bonds. It can induce charge delocalization, regulating the electronic structure of PtFe alloys and strengthening Pt–Fe coupling. The Pt-skin suppresses Fe dissolution, whereas the PtFe core optimizes oxygen reduction reaction (ORR) intermediate adsorption (e.g., *OH). Theoretical calculations confirm that the Fe atom adjusts the d-band center of the Pt atom, intensifying oxygen binding and shifting the rate-determining step. Electrochemically, PtFe–PA–NC achieves a half-wave potential of 0.85 V and retains 95.8% of specific energy density after more than 140 h in zinc-air batteries. In alkaline fuel cells, it delivers a peak power density of 508 mW cm−2 at an ultralow Pt loading (0.017 mg cm−2), approximately twice that of 5 wt% Pt/C (0.025 mg cm−2). This work showcases synergistic electronic and interfacial regulation through heteroatom doping and alloying, promoting high-performance hydrogen/metal air batteries.