Synergistic Pore Structure and Active Site Modulation in Co-N-C Catalysts Enabling Stable Zinc-Air Batteries

Development of cheap, highly active, and durable nonprecious metal-based oxygen electrocatalysts is essential for metal-air battery technology, but achieving the balance of oxygen evolution reaction (OER)/oxygen reduction reaction (ORR) bifunctional performance and long-term durability is still a great challenge. Using a typical Co-N-C catalyst as a model, herein, we introduced ammonium chloride into nitrogen-doped carbon materials containing metal elements during the pyrolysis process (Co-N-C/AC), which not only increases the active area but also realizes the accurate customization of the active site (pyridine nitrogen and cobalt oxide species) so as to achieve the balance of the OER/ORR bifunctional sites. The synthesized Co-N-C/AC bifunctional catalyst with a three-dimensional porous structure exhibits a smaller potential gap of 0.72 V. The peak power density of the aqueous cell at a current density of 308 mA cm^-2 is 203 mW cm^-2. The cycle life (≈3900 h) is longer than those of other recently reported aqueous Zn-air batteries (ZABs). The peak power density of the Co-N-C/AC-based quasi-solid-state ZAB reaches 550 mW cm^-2 for ∼72 h. This work shows a feasible path for the practical application of ZABs by balancing the bifunctional electrocatalysts by tailoring the active site reasonably.