In situ confinement of iron-based active sites within high porosity carbon frameworks with enhanced activity for rechargeable Zn–air battery

Non-noble bifunctional electrocatalysts with robust activity and stability toward oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) are greatly significant but challenging for Zn-air batteries. Here, in situ confinement of FeNx active sites in high porosity carbon framework (FeNx/CMCC) derived from chelate of carboxymethylcellulose (CMC) and iron ions were synthesized. Particularly, construction of FeNx within porous carbon framework accelerates the electron transfer and the sufficient utilization of active centers, and then expedites the reaction kinetics of ORR and OER. As expected, the optimized FeNx/CMCC exhibits superior ORR activity with a larger half-wave potential of 0.869 V. The rechargeable Zn-air battery delivers a higher power density of 99.6 mW/cm2 and a special capacity of 781.9 mA h/gZn at 10 mA/cm2, together with excellent durability of over 335 h. Remarkably, the as-assembled solid-state battery exhibits a higher open circuit voltage (OCV) of 1.5 V, a special capacity of 709.7 mA h/gZn, as well as prolonged cycling stability (90 h). Moreover, the flexible solid-state battery displays negligible loss of electrochemical performance under various bending angles, illustrating its potential application in flexible electronic devices.