In-Situ Nanoarchitectonics of Fe/Co LDH over Cobalt-Enriched N‑Doped Carbon Cookies as Facile Oxygen Redox Electrocatalysts for High-Rate Rechargeable Zinc–Air Batteries

The reality of long-term rechargeable and high-performance zinc–air batteries relies majorly on cost-effective and eminent bifunctional electrocatalysts, which can perform both the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER). Herein, we demonstrate a new approach for the synthesis of in-situ-grown layered double hydroxide of iron and cobalt over a cobalt nanoparticle-enriched nitrogen-doped carbon frame (CoL 2:1) by a simple coprecipitation reaction with facile scale-up and explore its electrocatalytic ORR and OER activity for an electrically rechargeable zinc–air battery. Consequently, the developed composite displays excellent ORR and OER activity with an ORR half-wave potential of 0.84 V, a limiting current density of 5.85 mA/cm2, and an OER overpotential of 320 mV with exceptional stability. The outstanding bifunctionality index of the catalyst (ΔE = 0.72 V) inspired us to utilize it as a cathode catalyst in an in-house developed prototype zinc–air battery. The battery could easily supply a specific capacity of 804 mAh/g with a maximum peak power density of 161 mW/cm2. The battery exhibits an attractive charge–discharge profile with a lesser voltage gap of 0.76 V at 10 mA/cm2 with durability for a period of 200 h and a voltage efficiency of 97%, which surpassed the corresponding Pt/C + RuO2-based zinc–air battery. Further, a maximum load of 50 mA/cm2 could easily be sustained during cycling, revealing its outstanding stability. A series-connected two CoL 2:1-based zinc–air batteries effortlessly enlighten a pinwheel fan and LED panel simultaneously, revealing its practicality. The high electrical conductivity and greater specific surface area of Co/N–C and its robust attachment with Fe/Co LDH preserves both active sites, thereby resulting in exceptional performance. Our method is capable of being flexible enough to create various bifunctional Co/N–C-based composite electrodes, opening up a feasible pathway to rechargeable zinc–air batteries with maximum energy density.