Solvent-Free Assembled Fe-Chitosan Chelates Derived N-Doped Carbon Layer-Encapsulated Fe/Fe3C for ORR and OER

Carbon encapsulated transition metal catalysts receive extensive attention in electrochemical catalytic oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) due to the unique structure and highly adjustable electronic configuration. Herein, we synthesized 3D porous Active-N-rich graphene-like carbon layer-encapsulated Fe/Fe3C (Fe@NCG) via pyrolysis of a mixture of solvent-free assembled Fe-chitosan chelates and additional small molecule nitrogen source urea, wherein space-confinement effect of chelates suppressed agglomeration of Fe3+ ions and small molecule nitrogen source facilitated regulation of N configurations. The optimized catalyst Fe@NCG shows remarkable ORR/OER bifunctional catalytic activity with a half-wave potential of 0.86 V for ORR and a moderate potential difference of 0.85 V in alkaline medium. Comparative studies revealed that Active-N-rich carbon layer and inner well-dispersed Fe/Fe3C nanoparticles and the favorable interface structures between them were responsible for high catalytic activity. Excitingly, the assembled zinc-air battery with Fe@NCG catalysts exhibits a high open-circuit potential (1.45 V), extremely high peak power density (204.50 mW/cm(2)) and energy density (814.70 Wh kg(-1)) as well as robust charge-discharge durability, surpassing those of noble metal catalyst. This proposed simple and universal strategy can also be extended to synthesize carbon encapsulated other transition metal electrocatalysts.