Manipulating the Electronic Structure of Graphite Intercalation Compounds for Boosting the Bifunctional Oxygen Catalytic Performance

Abstract Developing highly efficient bifunctional catalysts for the oxygen reduction and oxygen evolution reaction (ORR/OER) can open possibilities for future zinc air batteries (ZABs). Herein, cost‐effective and highly conductive few‐layer ferric and nickel chloride co‐intercalated graphite intercalation compounds (FeCl₃‐NiCl₂‐GIC) are designed as bifunctional oxygen catalysts for ZAB. The optimized few‐layer FeCl₃‐NiCl₂‐GIC catalyst exhibits a small overpotential of 276 mV at 10 mA cm^–2 for the OER and achieves a high onset potential of 0.89 V for the ORR. The theoretical analysis demonstrates the electron‐rich state on the carbon layers of FeCl₃‐NiCl₂‐GIC during the catalytic process favors the kinetics of electron transfer and lowers the absorption energy barriers for intermediates. Impressively, the ZAB assembled with few‐layer FeCl₃‐NiCl₂‐GIC catalyst displays a 160 h cycling stability and a high energy efficiency of 72.6%. This work also suggests the possibility of utilizing layer electronic structure regulation on graphite intercalation compounds as effective bifunctional catalysts for ZABs.