Regulating Fe-spin state by atomically dispersed Mn-N in Fe-N-C catalysts with high oxygen reduction activity

Gege Yang, Jiawei Zhu, Pengfei Yuan, Yongfeng Hu, Gan Qu, Bang-An Lu, Xiaoyi Xue, Hengbo Yin, Wenzheng Cheng, Junqi Cheng, Wenjing Xu, Jin Li, Jinsong Hu, Shichun Mu () and Jia-Nan Zhang ()
Additional contact information
Gege Yang: Zhengzhou University
Jiawei Zhu: Wuhan University of Technology
Pengfei Yuan: Zhengzhou University
Yongfeng Hu: Canadian Light Source
Gan Qu: Zhengzhou University
Bang-An Lu: Zhengzhou University
Xiaoyi Xue: Zhengzhou University
Hengbo Yin: Zhengzhou University
Wenzheng Cheng: Zhengzhou University
Junqi Cheng: Zhengzhou University
Wenjing Xu: Zhengzhou University
Jin Li: Zhengzhou University
Jinsong Hu: Chinese Academy of Sciences
Shichun Mu: Wuhan University of Technology
Jia-Nan Zhang: Zhengzhou University

Nature Communications, 2021, vol. 12, issue 1, 1-10

Abstract: Abstract 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.

Date: 2021
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DOI: 10.1038/s41467-021-21919-5

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