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Gege Yang, Jiawei Zhu, Pengfei Yuan, Yongfeng Hu, Gan Qu, Bang‐An Lu, Xiaoyi Xue, Yin Hengbo, Wenzheng Cheng, Junqi Cheng and 5 more
As low-cost electrocatalysts for oxygen reduction reaction applied to fuel cells and metal-air batteries, atomic-dispersed transition metal-nitrogen-carbon materials are emerging, but the genuine mechanism thereof is still arguable. Herein, by rational design and synthesis of dual-metal atomically dispersed Fe,Mn/N-C catalyst as model object, we unravel that the O2 reduction preferentially takes place on FeIII in the FeN4 /C system with intermediate spin state which possesses one eg electron (t2g4eg1) readily penetrating the antibonding π-orbital of oxygen. Both magnetic measurements and theoretical calculation reveal that the adjacent atomically dispersed Mn-N moieties can effectively activate the FeIII sites by both spin-state transition and electronic modulation, rendering the excellent ORR performances of Fe,Mn/N-C in both alkaline and acidic media (halfwave positionals are 0.928 V in 0.1 M KOH, and 0.804 V in 0.1 M HClO4), and good durability, which outperforms and has almost the same activity of commercial Pt/C, respectively. In addition, it presents a superior power density of 160.8 mW cm−2 and long-term durability in reversible zinc–air batteries. The work brings new insight into the oxygen reduction reaction process on the metal-nitrogen-carbon active sites, undoubtedly leading the exploration towards high effective low-cost non-precious catalysts.
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Yang, G., Zhu, J., Yuan, P., Hu, Y., Qu, G., Lu, B., Xue, X., Hengbo, Y., Cheng, W., Cheng, J., Xu, W., Li, J., Hu, J., Mu, S. C., & Zhang, J. (2021). Regulating Fe-spin state by atomically dispersed Mn-N in Fe-N-C catalysts with high oxygen reduction activity. Nature Communications, 12(1), 1734. https://doi.org/10.1038/s41467-021-21919-5
Yang, Gege, et al. "Regulating Fe-spin state by atomically dispersed Mn-N in Fe-N-C catalysts with high oxygen reduction activity." Nature Communications, vol. 12, no. 1, 2021, pp. 1734, https://doi.org/10.1038/s41467-021-21919-5.
Yang, Gege, Jiawei Zhu, Pengfei Yuan, Yongfeng Hu, Gan Qu, Bang‐An Lu, Xiaoyi Xue, et al. "Regulating Fe-spin state by atomically dispersed Mn-N in Fe-N-C catalysts with high oxygen reduction activity." Nature Communications 12, no. 1 (2021): 1734. https://doi.org/10.1038/s41467-021-21919-5.
Yang G., Zhu J., Yuan P. [и др.] Regulating Fe-spin state by atomically dispersed Mn-N in Fe-N-C catalysts with high oxygen reduction activity // Nature Communications. — 2021. — Vol. 12, № 1. — P. 1734. — URL: https://doi.org/10.1038/s41467-021-21919-5
@article{yang2021regulating,
title = {{Regulating Fe-spin state by atomically dispersed Mn-N in Fe-N-C catalysts with high oxygen reduction activity}},
author = {Gege Yang and Jiawei Zhu and Pengfei Yuan and Yongfeng Hu and Gan Qu and Bang‐An Lu and Xiaoyi Xue and Yin Hengbo and Wenzheng Cheng and Junqi Cheng and Wenjing Xu and Jin Li and Jin‐Song Hu and Shichun C. Mu and Jianan Zhang},
journal = {Nature Communications},
year = {2021},
volume = {12},
number = {1},
pages = {1734},
doi = {10.1038/s41467-021-21919-5},
url = {https://doi.org/10.1038/s41467-021-21919-5}
}TY - JOUR AU - Yang, Gege AU - Zhu, Jiawei AU - Yuan, Pengfei AU - Hu, Yongfeng AU - Qu, Gan AU - Lu, Bang‐An AU - Xue, Xiaoyi AU - Hengbo, Yin AU - Cheng, Wenzheng AU - Cheng, Junqi AU - Xu, Wenjing AU - Li, Jin AU - Hu, Jin‐Song AU - Mu, Shichun C. AU - Zhang, Jianan TI - Regulating Fe-spin state by atomically dispersed Mn-N in Fe-N-C catalysts with high oxygen reduction activity JO - Nature Communications VL - 12 IS - 1 SP - 1734 PY - 2021 DA - 2021/03/19 DO - 10.1038/s41467-021-21919-5 UR - https://doi.org/10.1038/s41467-021-21919-5 ER -
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