Edge-Site Engineering of Atomically Dispersed Fe-N4 by Selective C-N Bond Cleavage for Enhanced Oxygen Reduction Reaction Activities.
By Rui Jiang, Li Li, Tian Sheng, Gaofei Hu, Yueguang Chen, Leyu Wang. Journal of the American Chemical Society, 2018
676 citations recorded by the source corpus.
Single-atom metal-nitrogen-carbon (M-N-C) catalysts have sparked intense interests, but the catalytic contribution of N-bonding environment neighboring M-N4 sites lacks attention. Herein, a series of Fe-N-C nanoarchitectures have been prepared, which confer adjustable numbers of atomically dispersed Fe-N4 sites, tunable hierarchical micro-mesoporous structures and intensified exposure of interior active sites. The optimization between Fe-N4 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-N4 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.
Subfields: Electrical and Electronic Engineering, Materials Chemistry, Renewable Energy, Sustainability and the Environment
View Paper: https://www.semanticscholar.org/paper/2444eb859fd8b53a6229db78025df873a564ef79
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Citations in the corpus
- Atomically Dispersed Metal Catalysts for Oxygen Reduction (2019, methodology): “Reprinted with permission from Ref.(39), Copyright 2019, American Chemical Society.”