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[Display omitted] • A Zn 5 (OH) 6 (CO 3) 2 -assisted pyrolysis strategy is proposed to prepare a coupled catalyst. • Fe nanoparticles can optimize electronic structures and d-band center of Fe center. • Fe-FeN-C exhibits eminent ORR activity with a E 1/2 of 0.921 V in alkaline media. • The Zn-air batteries deliver high power density and long-cycle life for 408 h. Fe single-atom catalysts still suffer from unsatisfactory intrinsic activity and durability for oxygen reduction reaction (ORR). Herein, the coexisting Fe single atoms and nanoparticles on hierarchically porous carbon (denoted as Fe-FeN-C) are prepared via a Zn 5 (OH) 6 (CO 3) 2 -assisted pyrolysis strategy. Theoretical calculation reveals that the Fe nanoparticles can optimize the electronic structures and d-band center of Fe active center, hence reducing the reaction energy barrier for enhancing intrinsic activity. The Zn 5 (OH) 6 (CO 3) 2 self-sacrificial template not only can promote the formation of Fe single atoms, but also contributes to the construction of microporous/mesoporous/macroporous structures. Therefore, the obtained Fe-FeN-C exhibits impressive ORR activity with a half-wave potential of 0.921 V, which far exceeds Pt/C. With Fe-FeN-C as the cathode catalyst, the assembled Zn-air batteries delivered a maximum power density of 206 mW cm−2 and a long-cycle life over 400 h. [ABSTRACT FROM AUTHOR]

Atomically dispersed iron-nitrogen-carbon catalysts offer great potential in oxygen reduction reaction (ORR), yet the poor exposure and low density of Fe-N x sites causes relatively low ORR activity. Herein, a zinc-assisted MgO template strategy is reported to construct porous carbon-supported Fe-N 4 sites (Fe-N-C). Iron atoms surrounded by zinc species are converted to abundant Fe-N 4 sites rather than Fe containing nanoparticles. Meanwhile, both the zinc species and the MgO template can effectively produce porous structure so as to increase the utilization of Fe-N 4 sites. Fe-N-C achieves superior ORR performance and stability in alkaline medium. Theoretical calculations manifest that Fe-N 4 sites can narrow the energy barrier for ORR. Moreover, finite element simulation exhibits the porous framework in Fe-N-C could significantly accelerate the diffusion of O 2. Therefore, Fe-N-C provides a high peak power density and superior discharge ability toward Zn-air batteries. [Display omitted] • Atomically dispersed Fe-N-C are prepared by zinc-assisted template strategy. • High density of Fe-N x and hierarchical porosity boost oxygen reduction reaction. • The porous framework of Fe-N-C could significantly accelerate the diffusion of O 2. • The catalyst exhibits an excellent performance in Zn-air batteries. [ABSTRACT FROM AUTHOR]