Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 12, Issue 13, Pages 15271-15278Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c01206
Keywords
Fe-N-C single-atom catalysts; active site density; oxygen reduction reaction; density functional theory calculation; neighboring effects
Funding
- Ministry of Science and Technology of the People's Republic of China [2018YFA0208603, 2018YFA0208702, 2017YFA0303500]
- National Natural Science Foundation of China [21790351, 21703221, 21633006]
- Supercomputing Center of University of Science and Technology of China
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Exploring 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 (U-L) 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 similar to 4 angstrom apart. Further, under certain conditions, an otherwise unfavorable physisorbed-O(2-)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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