Nitrogen‐Doped Cobalt Pyrite Yolk–Shell Hollow Spheres for Long‐Life Rechargeable Zn–Air Batteries

Abstract Limited by the sluggish four‐electron transfer process, designing high‐performance nonprecious electrocatalysts for the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) is urgently desired for efficient rechargeable Zn–air batteries (ZABs). Herein, the successful synthesis of porous nitrogen‐doped cobalt pyrite yolk–shell nanospheres (N‐CoS 2 YSSs) is reported. Benefiting from the abundant porosity of the porous yolk–shell structure and unique electronic properties by nitrogen doping, the as‐prepared N‐CoS 2 YSSs possess more exposed active surface, thus giving rise to superior activity for reversible oxygen electrocatalysis and outstanding cycling stability (more than 165 h at 10 mA cm −2 ) in ZABs, exceeding the commercial Pt/C and RuO 2 hybrid catalysts. Moreover, the assembled ZABs, delivering a specific capacity of 640 mAh g Zn −1 , can be used for practical devices. This work provides a novel tactic to engineer sulfides as high efficiency and promising bifunctional oxygen electrocatalysts for advanced metal–air batteries.