Fe3C coupled with Fe-Nx supported on N-doped carbon as oxygen reduction catalyst for assembling Zn-air battery to drive water splitting

ABSTRACT Fe-N-C structures have been considered as a candidate to replace noble metal catalysts towards oxygen reduction reaction (ORR) due to their excellent electrocatalytic activity and durability. Herein, a zinc-mediated synthesis strategy is proposed for N-doped graphitic porous carbon encapsulated uniform dispersed Fe3C nanoparticles coupled with atomically dispersed Fe-Nx moieties (NPC/Fe-N-C) derived from biomass coconut shell. The introduction of zinc species could be conductive to the dispersion of iron species and formation of porous structures. Density functional theory calculations demonstrate that the N-doped carbon coating structures can weaken the oxygen intermediates adsorption energy barrier of Fe3C. Besides, the graphitic carbon could promote the electron transfer during the electrochemical reaction. These special structures enable NPC/Fe-N-C to have excellent ORR activity with an Eonset of 1.0 V, which is much better than Pt/C. Furthermore, the zinc-air battery assembled by pairing NPC/Fe-N-C with a high-efficiency oxygen evolution reaction (OER) catalyst can continuously and stably operate a charge-discharge potential gap of 0.8 V at 10 mA/cm2 for more than 600 hours. More importantly, the assembled batteries could drive overall water splitting device, realizing the effective energy conversion.