Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 140, Issue 37, Pages 11594-11598Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.8b07294
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Funding
- National Natural Science Foundation of China [21725501, 21475007, 21675009, 21701005]
- Fundamental Research Funds for the Central Universities [buctrc201812, buctrc201815]
- China Postdoctoral Science Foundation [2017M620583]
- Public Hatching Platform for Recruited Talents of Beijing University of Chemical Technology
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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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