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[Display omitted] • Novel CoSb/NC catalysts are prepared via a novel Sb-modulated strategy. • The feeding amount of Sb salt is tuned to modulate the particle size and pore structure of CoSb/NC catalysts. • CoSb/NC catalysts exhibit enhanced ORR activity and kinetics outperforming the state-of-the-art Pt/C. • CoSb/NC catalysts are electrocatalytically active toward OER. • CoSb/NC catalysts can drive rechargeable Zn-air battery with a high peak power density of 180 mW cm−2. Rational modulation and optimization of structural properties plays a significant role in advancing the electrocatalytic performance of electrocatalysts. In this study, we report a novel Sb-modulated strategy to synthesize novel CoSb/NC catalysts comprised of CoSb alloy supported on nitrogen-doped carbon (denoted as CoSb/NC). Apart from alloying with Co to generate CoSb alloys, we demonstrated that the evaporation of Sb could modulate the particle size and pore structure of CoSb/NC. Such modulation has facilitated the formation of micro/meso-porous structure to accelerate the mass/charge transport and increase the accessibility of active sites, resulting in a highest kinetic current density of 22.6 mA cm−2 at 0.85 V vs. RHE as well as a low Tafel slope of 38 mV dec−1, which even outperforms the state-of-the-art Pt/C. Additionally, CoSb/NC is demonstrated to be electrocatalytic active toward OER with the overpotential to be 430 mV at 10 mA cm−2. Rechargeable Zn-air battery tests reveal that CoSb/NC possesses competitive performance in terms of charge-discharge ability and stability, suggesting its potential application in renewable energy conversion devices. This work provides a novel approach to modulate the structure of nitrogen-doped carbon based materials as efficient oxygen electrocatalysts. [ABSTRACT FROM AUTHOR]

• Co/N-C Zn is prepared via high-temperature gas-transport approach. • The intrinsic structure of Co/ N-C Zn has been greatly modulated by ZnCl 2 treatment. • Co/N-C Zn exhibits enhanced ORR and OER performance. • ORR and OER active sites are determined by control experiments. • Co/N-C Zn can drive liquid and solid-state rechargeable Zn-air battery efficiently. In this study, a facile surface treatment on polypyrrole (PPy) nanofiber with ZnCl 2 solution is employed to fabricate N-doped carbon anchored with metallic Co (denoted as Co/N-C Zn) via gas-transport approach. Structural characterizations reveal that the intrinsic structure of Co/N-C Zn in terms of its morphology, pore structure and defects have been greatly modulated by such a surface treatment, resulting in a higher loading amount of metallic Co, larger surface area and increased pyridinic N and Co-N species as efficient active sites. Benefiting from the structural modulation, Co/N-C Zn exhibits outstanding ORR activity and kinetics with a positive half-wave potential of 0.88 V vs. RHE, a high kinetic current density (J k) value of 36.6 mA cm−2 at 0.85 V vs. RHE, and a small Tafel slope of 55.9 mV dec−1, which even outperforms commercial Pt/C. Moreover, enhanced OER performance is also achieved in Co/N-C Zn , with an overpotential of 280 mV at 10 mA cm−2, surpasses that of commercial RuO 2 (295 mV). Finally, Co/N-C Zn shows promise for substitution of commercial Pt/C and RuO 2 to drive both liquid and solid-state rechargeable Zn-air batteries with high peak power densities of 196 mW cm−2 and 130 mW cm−2. [ABSTRACT FROM AUTHOR]