Co@Co3O4 Encapsulated in Carbon Nanotube‐Grafted Nitrogen‐Doped Carbon Polyhedra as an Advanced Bifunctional Oxygen Electrode

Abstract Efficient reversible oxygen electrodes for both the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) are vitally important for various energy conversion devices, such as regenerative fuel cells and metal–air batteries. However, realization of such electrodes is impeded by insufficient activity and instability of electrocatalysts for both water splitting and oxygen reduction. We report highly active bifunctional electrocatalysts for oxygen electrodes comprising core–shell Co@Co 3 O 4 nanoparticles embedded in CNT‐grafted N‐doped carbon‐polyhedra obtained by the pyrolysis of cobalt metal–organic framework (ZIF‐67) in a reductive H 2 atmosphere and subsequent controlled oxidative calcination. The catalysts afford 0.85 V reversible overvoltage in 0.1 m KOH, surpassing Pt/C, IrO 2 , and RuO 2 and thus ranking them among one of the best non‐precious‐metal electrocatalysts for reversible oxygen electrodes.