MOF-Derived Co and Fe Species Loaded on N-Doped Carbon Networks as Efficient Oxygen Electrocatalysts for Zn-Air Batteries

HIGHLIGHTS: A novel method is developed to prepare bifunctional oxygen electrocatalysts composed of Co nanoparticles and highly dispersed Fe loaded on N-doped carbon substrates by virtues of metal-organic frameworks and two different doping processes. The designed catalysts show comparable performance with commercial catalysts. Meanwhile, rechargeable Zn-air batteries with prepared catalysts demonstrate high peak power density and good cycling stability. The performance promotion originates from the synergy between Co nanoparticles and highly dispersed Fe, porous structures, large specific areas, and distinct three-dimensional carbon networks. . ABSTRACT: Searching for cheap, efficient, and stable oxygen electrocatalysts is vital to promote the practical performance of Zn-air batteries with high theoretic energy density. Herein, a series of Co nanoparticles and highly dispersed Fe loaded on N-doped porous carbon substrates are prepared through a “double-solvent” method with in situ doped metal-organic frameworks as precursors. The optimized catalysts exhibit excellent performance for oxygen reduction and evolution reaction. Furthermore, rechargeable Zn-air batteries with designed catalysts demonstrate higher peak power density and better cycling stability than those with commercial Pt/C+RuO(2). According to structure characterizations and electrochemical tests, the interaction of Co nanoparticles and highly dispersed Fe contributes to the superior performance for oxygen electrocatalysis. In addition, large specific surface areas, porous structures and interconnected three-dimensional carbon networks also play important roles in improving oxygen electrocatalysis. This work provides inspiration for rational design of advanced oxygen electrocatalysts and paves a way for the practical application of rechargeable Zn-air batteries. [Image: see text] SUPPLEMENTARY INFORMATION: The online version contains supplementary material available at 10.1007/s40820-022-00890-w.