Edge-Site Engineering of Atomically Dispersed Fe-N4 by Selective C-N Bond Cleavage for Enhanced Oxygen Reduction
Rui Jiang1, Li Li1, Tian Sheng2
1State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Center for Soft Matter Science and Engineering , Beijing University of Chemical Technology , Beijing 100029 , China.
Abstract:
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.
More Related Videos
10:57Synthesis and Performance Characterizations of Transition Metal Single Atom Catalyst for Electrochemical CO2 Reduction
Published on: April 10, 2018
08:57Scalable Syntheses of Graphene Oxide and Reduced Graphene Oxide using Cascade Design Oxidation and Highly Basic Reduction Reactions
Published on: July 3, 2025
Related Concept Videos
C–C Bond Cleavage: Retro-Aldol Reaction
In the first step, as depicted in Figure 1, the base deprotonates the β-hydroxy ketone at the hydroxyl group to form an alkoxide ion.
Oxidation-Reduction Reactions
Metal-Ligand Bonds
In these complexes, transition metals form coordinate covalent bonds, a kind of Lewis acid-base interaction in which both of the electrons in the bond are contributed by a donor (Lewis base) to an electron acceptor (Lewis acid). The Lewis acid in...
Bond Energies and Bond Lengths
Bonding in Metals
Phase I Reactions: Reductive Reactions
