Journal
ADVANCED MATERIALS
Volume 34, Issue 29, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202202544
Keywords
axial charge redistribution; d-band center; electrocatalysis; Fe single-atom catalysts; oxygen reduction reaction
Categories
Funding
- James Cook Research Fellowship
- MacDiarmid Institute for Advanced Materials and Nanotechnology
- Energy Education Trust of New Zealand
- National Key Projects for Fundamental Research and Development of China [2018YFB1502002]
- National Natural Science Foundation of China [51825205, 51772305, 21871279, 21902168]
- Beijing Natural Science Foundation [2191002]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDB17000000]
- Royal Society-Newton Advanced Fellowship [NA170422]
- K. C. Wong Education Foundation
- Youth Innovation Promotion Association of the CAS
- International Partnership Program of Chinese Academy of Sciences [GJHZ201974]
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This study reports the development of FeN4-O-NCR catalysts with excellent intrinsic activity for alkaline ORR by optimizing the intrinsic ORR activity of Fe single-atom sites. The catalyst demonstrates outstanding performance in electrochemical tests, outperforming existing catalysts, and exhibits high power density when used in a zinc-air battery.
Fe-N-C catalysts offer excellent performance for the oxygen reduction reaction (ORR) in alkaline media. With a view toward boosting the intrinsic ORR activity of Fe single-atom sites in Fe-N-C catalysts, fine-tuning the local coordination of the Fe sites to optimize the binding energies of ORR intermediates is imperative. Herein, a porous FeN4-O-NCR electrocatalyst rich in catalytically accessible FeN4-O sites (wherein the Fe single atoms are coordinated to four in-plane nitrogen atoms and one subsurface axial oxygen atom) supported on N-doped carbon nanorods (NCR) is reported. Fe K-edge X-ray absorption spectroscopy (XAS) verifies the presence of FeN4-O active sites in FeN4-O-NCR, while density functional theory calculations reveal that the FeN4-O coordination offers a lower energy and more selective 4-electron/4-proton ORR pathway compared to traditional FeN4 sites. Electrochemical tests validate the outstanding intrinsic activity of FeN4-O-NCR for alkaline ORR, outperforming Pt/C and almost all other M-N-C catalysts reported to date. A primary zinc-air battery constructed using FeN4-O-NCR delivers a peak power density of 214.2 mW cm(-2) at a current density of 334.1 mA cm(-2), highlighting the benefits of optimizing the local coordination of iron single atoms.
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