4.6 Article

Spin state modulation on dual Fe center by adjacent Ni sites enabling the boosted activities and ultra-long stability in Zn-air batteries

期刊

SCIENCE BULLETIN
卷 68, 期 18, 页码 2042-2053

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ELSEVIER
DOI: 10.1016/j.scib.2023.07.049

关键词

Dual-metal-atom; Electron spin state; Oxygen reduction reaction; Rechargeable stability

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This study deliberately constructs Fe/Ni-NHCS as an ORR catalyst, which achieves excellent ORR performance and ultra-long-term stability by optimizing the electron spin state and reducing the energy barrier. It opens up a new avenue for energy conversion technologies.
Breakthrough in developing cost-effective Fe-based catalysts with superior oxygen reduction reaction (ORR) activities and ultra-long-term stability for application in Zn-air batteries (ZABs) remain a priority but still full of challenges. Herein, the neighboring NiN4 single-metal-atom and Fe2N5 dual-metal-atoms on the N-doped hollow carbon sphere (Fe/Ni-NHCS) were deliberately constructed as the efficient and robust ORR catalyst for ZABs. Both theory calculations and magnetic measurements demonstrate that the introduction of NiN4 provides a significant role on optimizing the electron spin state of Fe2N5 sites and reducing the energy barrier for the adsorption and conversion of the oxygen-containing intermediates, enabling the Fe/Ni-NHCS with excellent ORR performance and ultralow byproduct HO2 yield (0.5%). Impressively, the ZABs driven by Fe/Ni-NHCS exhibit unprecedented long-term rechargeable stability over 1200 h. This work paves a new venue to manipulate the spin state of active sites for simultaneously achieving superior catalytic activities and ultra-long-term stability in energy conversion technologies. (C) 2023 Science China Press. Published by Elsevier B.V. and Science China Press. All rights reserved.

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