Stable confinement of Fe/Fe3C in Fe, N-codoped carbon nanotube towards robust zinc-air batteries

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Catalytic oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) have garnered great attention as the key character in metal-air batteries. Herein, we developed a superior nonprecious bifunctional oxygen electrocatalyst, fabricated through spatial confinement of Fe/Fe3C nanocrystals in pyridinic N and Fe-Nx rich carbon nanotubes (Fe/Fe3C-N-CNTs). During ORR, the resultant electrocatalyst exhibits positive onset potential of 1.0 V (vs. RHE), large half-wave potentials of 0.88 V (vs. RHE), which is more positive than Pt/C (0.98 V and 0.83 V, respectively). Remarkably, Fe/Fe3C-N-CNTs exhibits outstanding durability and great methanol tolerance, exceeding Pt/C and most reported nonprecious metal-based oxygen reduction electrocatalysts. Moreover, Fe/Fe3C-N-CNTs show a markedly low potential at j=10 mA/cm2, small Tafel slopes and extremely high stability for OER. Impressively, the Fe/Fe3C-N-CNTs-based Zn-air batteries demonstrate high power density of 183 mW/cm2 and robust charge/discharge stability. It is revealed that the spatial confinement effect can impede the aggregation and corrosion of Fe/Fe3C nanocrystals. Meanwhile, Fe/Fe3C and Fe-Nx play synergistic effect on boosting the ORR/OER activity, which provides an important guideline for construction of inexpensive nonprecious metal-carbon hybrid nanomaterials.
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