Interfacing Manganese Oxide and Cobalt in Porous Graphitic Carbon Polyhedrons Boosts Oxygen Electrocatalysis for Zn–Air Batteries

Rational design and synthesis of highly active and robust bifunctional non‐noble electrocatalysts for both oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) are urgently required for efficient rechargeable metal–air batteries. Herein, abundant MnO/Co heterointerfaces are engineered in porous graphitic carbon (MnO/Co/PGC) polyhedrons via a facile hydrothermal‐calcination route with a bimetal–organic framework as the precursor. The in situ generated Co nanocrystals not only create well‐defined heterointerfaces with high conductivity to overcome the poor OER activity but also promote the formation of robust graphitic carbon. Owing to the desired composition and formation of the heterostructures, the resulting MnO/Co/PGC exhibits superior activity and stability toward both OER and ORR, which makes it an efficient air cathode for the rechargeable Zn–air battery. Importantly, the homemade Zn–air battery is able to deliver excellent performance including a peak power density of 172 mW cm^?2 and a specific capacity of 872 mAh g^?1, as well as excellent cycling stability (350 cycles), outperforming commercial mixed Pt/C||RuO₂ catalysts. This work highlights the synergy from heterointerfaces in oxygen electrocatalysis, thus providing a promising approach for advanced metal–air cathode materials.