Fe, N‐Inducing Interfacial Electron Redistribution in NiCo Spinel on Biomass‐Derived Carbon for Bi‐functional Oxygen Conversion

Herein, an interfacial electron redistribution is proposed to boost the activity of carbon-supported spinel NiCo2O4 catalyst toward oxygen conversion via Fe, N-doping strategy. Fe-doping into octahedron induces a redistribution of electrons between Co and Ni atoms on NiCo1.8Fe0.2O4@N-carbon. The increased electron density of Co promotes the coordination of water to Co sites and further dissociation. The generation of proton from water improves the overall activity for the oxygen reduction reaction (ORR). The increased electron density of Ni facilitates the generation of oxygen vacancies. The Ni-VO-Fe structure accelerates the deprotonation of *OOH to improve the activity toward oxygen evolution reaction (OER). N-doping modulates the electron density of carbon to form active sites for the adsorption and protonation of oxygen species. Fir wood-derived carbon endows catalyst with an integral structure to enable outstanding electrocatalytic performance. The NiCo1.8Fe0.2O4@N-carbon express high half-wave potential up to 0.86 V in ORR and low overpotential of 270 mV at 10 mA cm-2 in OER. The zinc-air batteries (ZABs) assembled with the as-prepared catalyst achieve long-term cycle stability (over 2000 cycles) with peak power density (180 mWcm-2). Fe, N-doping strategy drives the catalysis of biomass-derived carbon-based catalysts to the highest level for the oxygen conversion in ZABs.