am0c01206_si_001.pdf (3.74 MB)
Impact of Active Site Density on Oxygen Reduction Reactions Using Monodispersed Fe–N–C Single-Atom Catalysts
journal contribution
posted on 2020-03-19, 14:05 authored by Yulan Han, Qin-Kun Li, Ke Ye, Yi Luo, Jun Jiang, Guozhen ZhangExploring the impact
of active site density on catalytic reactions is crucial for reaching
a more comprehensive understanding of how single-atom catalysts work.
Utilizing density functional theory calculations, we have systematically
investigated the neighboring effects between two adjacent Fe–N–C
sites of monodispersed Fe–N–C single-atom catalysts
on oxygen reduction reaction (ORR). While the thermodynamic limiting
potential (UL) is strongly dependent on
the intersite distance and the nature of adjacent active sites in
FeN3, it is almost invariable in FeN4 until
two FeN4 sites are ∼4 Å apart. Further, under
certain conditions, an otherwise unfavorable physisorbed-O2-initiated 2e– pathway becomes feasible due to
charge transfer between reactive species and graphene support. Our
results cast new insight into the rational design of high-density
single-atom catalysts and may create an alternative route to manipulate
their catalytic activities.
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graphene supportFeN 4alternative routetheory calculationsimpactphysisorbed-O 2reactive speciesresults castFeN 3charge transferOxygen Reduction ReactionsActive Site DensityU Loxygen reduction reactionsingle-atom catalystssingle-atom catalysts workUtilizing densityORRintersite distancesite densityFeN 4 sites
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