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Rational design of highly effective and low-cost oxygen reduction reaction (ORR) electrocatalysts to replace Pt-based catalysts is still a significant challenge for rechargeable zinc-air batteries. Hence, Fe, N co-doped one-dimensional carbon nanofibers with Fe 4 N species (Fe/N-CNFs) are synthesized through the electrospun technique combining with the "rapid calcination under vacuum" method. Benefitting from the one-dimensional structure obtained by the electrospun technique, the as-synthesized Fe/N-CNFs electrocatalyst with mesoporous exhibits a relatively large specific surface area of 624.12 m2 g−1. Notably, the intrinsic activity of Fe 4 N species as well as the large specific surface area can endow the resulting Fe/N-CNFs with a positive half-wave potential of 0.88 V compared with 20 wt% Pt/C (0.86 V) for ORR. The Fe/N-CNFs also exhibits better long-term stability than 20 wt% Pt/C. Furthermore, the rechargeable zinc-air battery constructed with Fe/N-CNFs as the cathode shows a high open-circuit voltage of 1.51 V, a peak power density of 135 mW cm−2 and an excellent cycle life for 55 h. The as-synthesized electrocatalyst is promising to replace the precious metal catalysts for rechargeable zinc-air batteries. Unlabelled Image • Fe, N co-doped carbon nanofibers (Fe/N-CNFs) with Fe 4 N species were synthesized. • The "rapid calcination under vacuum" was reported for the preparation of Fe/N-CNFs. • The one-dimensional structure of Fe/N-CNFs provides a large specific surface area. • The Fe/N-CNFs exhibits more excellent ORR activity than commercial 20 wt% Pt/C. • The Fe/N-CNFs endows zinc-air batteries with comparable performances to 20 wt% Pt/C. [ABSTRACT FROM AUTHOR]

The in-situ immobilization of Co/MnO hetero-nanoparticles onto N,S co-doped carbon nanotubes/nanofiber-integrated hierarchical branched superstructures demonstrates excellent oxygen reduction electrocatalytic activity, stability and performs robust cycling stability. [Display omitted] • The Co/MnO hetero-nanoparticles were immobilized onto carbon nanofibers. • The heterojunctions cause electronic redistribution and create more active sites. • The "branches"/"trunk"-structure could accelerate electrolyte and mass transport. • The Co/MnO@N,S-C NT/NFs-equipped Zn-air battery shows superior cycling stability. Electronic regulation via interfacial formation is identified as a versatile strategy to improve the electrocatalytic activity. Herein, we report a feasible electrospinning-pyrolysis approach for the in-situ immobilization of Co/MnO hetero-nanoparticles onto N,S co-doped carbon nanotubes/nanofiber-integrated hierarchical branched superstructures (abbreviated as Co/MnO@N,S-C NT/CNFs hereafter). The simultaneous realization of interfacial engineering and nanocarbon hybridization renders the fabricated Co/MnO@N,S-C NT/CNFs with abundant firmly anchored active sites, modified electronic configuration, improved electric conductivity, efficient mass transport pathways, and significantly reinforced stability. Profiting from the compositional synergy and architectural advantages, the Co/MnO@N,S-C NT/CNFs exhibit outstanding ORR activity, superior tolerance to methanol, and excellent long-term stability in KOH electrolyte. More encouragingly, as a proof-of-concept demonstration, the rechargeable aqueous and flexible all-solid-state Zn-air batteries using Co/MnO@N,S-C NT/NFs + RuO 2 as the air-cathode afford higher power densities, larger specific capacities and superb cycling stability, outperforming the state-of-the-art Pt/C + RuO 2 counterparts. This work demonstrates the great contribution of heterointerfaces for oxygen electrocatalysis. [ABSTRACT FROM AUTHOR]