Fe-NC@NiFe-LDH Derived from Iron-Based Metal–Organic Frameworks as an Efficient Bifunctional Oxygen Electrocatalyst for Zn–Air Batteries

The rational design and synthesis of efficient and durable bifunctional electrocatalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is of great significance and challenging for rechargeable zinc–air batteries. While much attention has been devoted to enhancing ORR performance in recent studies, the effectiveness of OER is equally crucial for charging performance of Zn–air batteries. In this work, NH2-MIL-101(Fe) is employed as a precursor to derive Fe-NC through a straightforward pyrolysis method. Subsequently, NiFe-LDH is synthesized on the surface of Fe-NC via a wet-chemical process to obtain Fe-NC@NiFe-LDH. Capitalizing on the synergistic interplay between Fe-NC, serving as the ORR active site, and NiFe-LDH, acting as the OER active site, Fe-NC@NiFe-LDH demonstrates remarkable bifunctional electrocatalytic performance, boasting a positive half-wave potential of 0.83 V for ORR and a low potential of 1.68 V for OER at a current density of 10 mA cm−2, alongside exceptional stability in alkaline environments. Furthermore, the Fe-NC@NiFe-LDH-based Zn–air battery exhibits outstanding discharge and charge performance, maintaining excellent cycling stability over 600 h (3600 cycles).