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- Title
Regulating Fe-spin state by atomically dispersed Mn-N in Fe-N-C catalysts with high oxygen reduction activity.
- Authors
Yang, Gege; Zhu, Jiawei; Yuan, Pengfei; Hu, Yongfeng; Qu, Gan; Lu, Bang-An; Xue, Xiaoyi; Yin, Hengbo; Cheng, Wenzheng; Cheng, Junqi; Xu, Wenjing; Li, Jin; Hu, Jinsong; Mu, Shichun; Zhang, Jia-Nan
- 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. The working mechanism of several low-cost electrocatalyst materials is still arguable. Here the authors show a model Fe,Mn/N-C catalyst where the oxygen reduction preferentially takes place on Fe(III) sites with the intermediate spin state (t2g4 eg1) caused by the adjacent Mn-N moieties.
- Subjects
PRECIOUS metals; OXYGEN reduction; ELECTROCATALYSTS; METAL-air batteries; ELECTRONIC modulation; CATALYSTS; POWER density; MAGNETIC measurements
- Publication
Nature Communications, 2021, Vol 12, Issue 1, p1
- ISSN
2041-1723
- Publication type
Article
- DOI
10.1038/s41467-021-21919-5