Facile Synthesis of Vertical Layered Double Hydroxides Nanosheets on Co@Carbon Nanoframes as Robust Bifunctional Oxygen Electrocatalysts for Rechargeable Zn–Air Batteries

The development of efficient and low‐cost bifunctional catalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is imperative but remains challenging in rechargeable zinc–air batteries. Herein, a metal oxidation‐assisted approach is developed for the facile synthesis of a highly efficient bifunctional catalyst (Co@NC@LDHs) which is composed of layered double hydroxides (LDHs) nanosheets in situ vertically grown on the surface of hollow carbon nanoframes encapsulating Co nanoparticles (Co@NC). Specifically, the vertical LDHs distributing on the carbon surface ensure the maximized number of accessible active sites and the interaction between LDHs with the carbon matrix. The hierarchically structured bifunctional Co@NC@LDHs display an overpotential of 0.33 V at 10 mA cm −2 for OER and a half‐wave potential of 0.88 V for ORR. The potential gap (Δ E ) of Co@NC@LDHs is calculated to be 0.68 V, outperforming the mixed Pt/C + RuO 2 catalysts (Δ E = 0.77 V), manifesting its superior bifunctional electrocatalysis performance. Moreover, the Zn–air batteries based on Co@NC@LDHs electrocatalyst exhibit a high peak power density (185.2 mW cm −2 ) and excellent durability (5.0 mA cm −2 over 500 h). This work may provide a facile strategy for the fabrication of LDHs on carbon substrate, acting as efficient catalysts for broad energy‐related applications.