Edge-Site Engineering of Atomically Dispersed Fe–N4 by Selective C–N Bond Cleavage for Enhanced Oxygen Reduction Reaction Activities
Abstract
Single-atom metal-nitrogen-carbon (M-N-C) catalysts have sparked intense interests, but the catalytic contribution of N-bonding environment neighboring M-N 4 sites lacks attention. Herein, a series of Fe-N-C nanoarchitectures have been prepared, which confer adjustable numbers of atomically dispersed Fe-N 4 sites, tunable hierarchical micro-mesoporous structures and intensified exposure of interior active sites. The optimization between Fe-N 4 single sites and carbon matrix delivers superior oxygen reduction reaction activity (half-wave potential of 0.915 V vs RHE in alkaline medium) with remarkable stability and high atom-utilization efficiency (almost 10-fold enhancement). Both experiments and theoretical calculations verified the selective C-N bond cleavage adjacent to Fe center induced by porosity engineering could form edge-hosted Fe-N 4 moieties, and therefore lower the overall oxygen reduction reaction barriers comparing to intact atomic configuration. These findings provide a new pathway for the integrated engineering of geometric and electronic structures of single-atom materials to improve their catalytic performance.
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Single metal atom sites at micropores and nanowrinkles often entail an asymmetrical coordination shell compared to single atom sites on a basal plane.
“More importantly, the single metal atom sites at the micropores and nanowrinkles often entail an asymmetrical coordination shell, as compared to single atom sites on a basal plane [44,47].”
From Atomically dispersed ruthenium in carbon aerogels as effective catalysts for pH-universal hydrogen evolution reaction (2022) · cites this paper as [47]
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High-Performance Electrocatalysts for Oxygen Reduction Derived from Polyaniline, Iron, and Cobalt
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Single atom electrocatalysts supported on graphene or graphene-like carbons
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- Authors
- Jiang, R., Li, L., Sheng, T., Hu, G., Chen, Y., & Wang, L.
- Affiliations
- State Key Laboratory of Chemical Resource Engineering (CN)
- Anhui Normal University (CN)
- Corresponding author
- Chen, Yueguang
- Wang, Leyu
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2018-08-31
- Volume
- 140
- Issue
- 37
- Pages
- 11594-11598
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2888882000
- Cited by
- 797
- References
- 2
- Citations by year
- 2026: 39 · 2025: 74 · 2024: 101 · 2023: 105 · 2022: 125 · 2021: 142 · 2020: 140 · 2019: 70 · 2018: 1
- FWCI
- 20.40
- Type
- journal article
- Language
- en
- Open access
- closed
- Licence
- Locations
- Journal of the American Chemical Society (publishedVersion)
- PubMed (publishedVersion)
- Funders
- Ministry of Education of the People's Republic of China (buctrc201812, buctrc201815)
- China Postdoctoral Science Foundation (2017M620583)
- Beijing University of Chemical Technology
- National Natural Science Foundation of China (21475007, 21675009, 21701005, 21725501)
- Topics
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
- Physical Sciences › Materials Science › Materials Chemistry › Catalytic Processes in Materials Science
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
- Keywords
- Fe-N4 single-atom catalysts, oxygen reduction reaction, C–N bond cleavage, porosity engineering, atom utilization efficiency, alkaline electrocatalysis, metal-nitrogen-carbon catalysts
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