Abstract

As a promising energy conversion and storage device, recently, rechargeable zinc-air batteries (ZABs) have developed rapidly, and the exploitation of excellent electrode catalysts to improve the energy efficiency and long-term performance of ZABs has become a focus of current research. Herein, the Co5.47N nanocrystals embedded in porous carbon nanofibers (Co5.47N PCNFs) were designed to act as a bifunctional electrocatalyst for the oxygen reduction reaction (ORR) and iodide oxidation reaction (IOR), which occur on the electrode in the charging-discharging process of ZABs. The electrochemistry results showed that the ORR activity of Co5.47N PCNFs is comparable to the commercial Pt/C electrocatalyst, and the IOR activity and stability are higher than those of the Pt/C electrocatalyst. Importantly, Co5.47N PCNFs electrocatalyst endows ZABs with a low charge–discharge voltage difference (0.49 V), a high round-trip energy efficiency (72.1 %), as well as a large specific capacity (791.5 mAh gZn−1), surpassing the performance of Pt/C electrocatalyst. Density functional theory calculation demonstrates that Co5.47N PCNFs have lower Gibbs free energy for the formation of IOR intermediate species, thereby displaying outstanding IOR catalytic performance compared to that of Pt/C electrocatalyst. These findings offer crucial insights into the rational design of cobalt nitride-based electrocatalysts for application in ZABs with high energy efficiency.

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