In:
ChemPhysChem, Wiley, Vol. 24, No. 16 ( 2023-08-15)
Kurzfassung:
Electrochemical reactions mostly take place at a constant potential, but traditional DFT calculations operate at a neutral charge state. In order to really model experimental conditions, we developed a fixed‐potential simulation framework via the iterated optimization and self‐consistence of the required Fermi level. The B‐doped graphene‐based FeN 4 sites for oxygen reduction reaction were chosen as the model to evaluate the accuracy of the fixed‐potential simulation. The results demonstrate that *OH hydrogenation gets facile while O 2 adsorption or hydrogenation becomes thermodynamically unfavorable due to the lower d‐band center of Fe atoms in the constant potential state than the neutral charge state. The onset potential of ORR over B‐doped FeN 4 by performing potential‐dependent simulations agree well with experimental findings. This work indicates that the fixed‐potential simulation can provide a reasonable and accurate description on electrochemical reactions.
Materialart:
Online-Ressource
ISSN:
1439-4235
,
1439-7641
DOI:
10.1002/cphc.202300152
Sprache:
Englisch
Verlag:
Wiley
Publikationsdatum:
2023
ZDB Id:
2025223-7
