A Bifunctional Iron‐Nickel Oxygen Reduction/Oxygen Evolution Catalyst for High‐Performance Rechargeable Zinc–Air Batteries

Abstract Efficient and robust electrocatalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are crucial for fuel cells, metal‐air batteries, and other energy technologies. Here, a highly stable, efficient bifunctional OER/ORR electrocatalyst (FeNi‐NC@MWCNTs) is reported and demonstrated its integration and robust performance in an aqueous Zinc–air battery (ZAB). The catalyst is based on neighboring iron/nickel sites (FeNiN 6 ) which are atomically dispersed on porous nitrogen‐doped carbon particles. The particles are wrapped in electrically conductive multi‐walled carbon nanotubes for enhanced electrical conductivity. Electrocatalytic analyses show high OER and ORR performance (OER/ORR voltage difference = 0.69 V). Catalyst integration in a ZAB results in excellent performance metrics, including an open circuit voltage of 1.44 V, a specific capacity of 782 mAh g −1 (at j = 15 mA cm −2 ), a peak power density of 218 mW cm −2 (at j = 260 mA cm −2 ) and long‐term durability over 600 charge/discharge cycles. Combined experimental and theoretical (density functional theory) analyses provide an in‐depth understanding of the physical and electronic structure of the catalyst and the role of the FeNi dual atom reaction site. The study therefore provides critical insights into the structure and reactivity of high‐performance bifunctional OER/ORR catalysts based on atomically dispersed non‐critical metals.