Regulating the spin state of triple-atom catalysts for improved oxygen electrocatalysis in zinc-air batteries at subzero temperature

Canhui Zhang; Zhuangzhuang He; Li Qiao; Xu Liu; Kaiyue Chen; Xingkun Wang; Jian Zhou; Lei Chu; Guanghui Wang; Minghua Huang; Heqing Jiang

doi:10.59717/j.xinn-mater.2025.100131

The Innovation Materials > 2025 Vol. 3 > No. 2 > 100131

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Regulating the spin state of triple-atom catalysts for improved oxygen electrocatalysis in zinc-air batteries at subzero temperature

1.
School of Materials Science and Engineering, Ocean University of China, Qingdao 266100, China
2.
Key Laboratory of Photoelectric Conversion and Utilization of Solar Energy, Qingdao New Energy Shandong Laboratory, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao, China
3.
These authors contributed equally

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Corresponding authors: huangminghua@ouc.edu.cn (M.H.); chulei@ouc.edu.cn (L.C.); xingkunwang@163.com (X.W.); jianghq@qibebt.ac.cn (H.J.)
Received Date: November 06, 2024

Accepted Date: April 21, 2025

Published Online: May 06, 2025

The Innovation Materials 3(2), https://doi.org/10.59717/j.xinn-mater.2025.100131 | Cite this article

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PUBLIC SUMMARY

PUBLIC SUMMARY
1. Single CoN₄ site was introduced to modulate the spin state of dual-atom Fe₂N₅.
  
  The Fe₂/Co-NHCS with medium spin state demonstrates excellent oxygen reduction reaction performance.
  
  Zinc-air batteries powered by Fe₂/Co-NHCS demonstrate superior performance at normal and low temperature.

ABSTRACT

ABSTRACT

Triple-atom catalysts (TACs), building upon dual-atom catalysts, have demonstrated exceptional catalytic activity toward oxygen reduction reaction (ORR). Nevertheless, advancing the catalytic activity of TACs for application in low-temperature (Low-T) energy conversion devices remains a formidable challenge, primarily limited by the slow capture efficiency of oxygen reactants at catalytic sites. In this work, utilizing Fe-Fe double atomic pairs as a foundational research model, we plant the CoN₄ site adjacent to activate them to construct efficient ORR electrocatalysts (named as Fe₂/Co-NHCS) featuring the Fe₂N₅+CoN₄ tri-atomic structure. The adjacent CoN₄ site can optimize the spin state of the Fe-Fe double atomic pairs from low to medium spin with ${ {t}_{{2g}^{4}}} $ ${ {e}_{{g}^{1}} }$3d-electron configuration, which makes the catalysts bind with oxygen reactants more readily to complete ORR process. As anticipated, the Fe₂/Co-NHCS achieved a high half-wave potential of 0.92 V. Moreover, the flexible Zn-air batteries powered by Fe₂/Co-NHCS deliver a large peak power density of 57.3 mW cm^-2 and brilliant charge-discharge stability over 150 stable cycles at -40°C. This research advances ORR electrocatalysts by modulating the electron spin states at diatomic Fe sites, paving a viable route for expanding the application range of ZABs in low-temperature environment.
- Triple atom catalysts /
- Zinc-air batteries /
- Electron spin state /
- Oxygen reduction reaction /
- Low-temperature application

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Zhang C., He Z., Qiao L., et al. (2025). Regulating the spin state of triple-atom catalysts for improved oxygen electrocatalysis in zinc-air batteries at subzero temperature. The Innovation Materials 3:100131. https://doi.org/10.59717/j.xinn-mater.2025.100131

Zhang C., He Z., Qiao L., et al. (2025). Regulating the spin state of triple-atom catalysts for improved oxygen electrocatalysis in zinc-air batteries at subzero temperature. The Innovation Materials 3:100131. https://doi.org/10.59717/j.xinn-mater.2025.100131

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Regulating the spin state of triple-atom catalysts for improved oxygen electrocatalysis in zinc-air batteries at subzero temperature

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