Abstract
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 Zn5(OH)6(CO3)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 Zn5(OH)6(CO3)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.
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