Samenvatting
Iron-nitrogen-carbon materials have been known as the most promising non-noble metal catalyst for proton-exchange membrane fuel cells (PEMFCs), but the genuine active sites for oxygen reduction reaction (ORR) are still arguable. Herein, by the thorough density functional theory investigations, we unravel that the planar Fe2N6 site exhibits excellent ORR catalytic activity over both FeN3 and FeN4 sites, and the potential-determining step is determined to be the *OH hydrogenation step with an overpotential of 0.415 V. The ORR activity of Fe2N6 site originates from the low spin magnetic moment (1.11 μB), which leads to high antibonding states and low d-band center of the Fe center, further leads to weak binding strength of *OH species. The density of FeN4 sites only has little influence on the ORR activity owing to the similar interaction between active site and intermediates in ORR. Our research sheds light on the activity origin of iron-nitrogen-carbon materials for ORR.
| Originele taal-2 | Engels |
|---|---|
| Artikelnummer | e202200165 |
| Aantal pagina's | 5 |
| Tijdschrift | ChemPhysChem |
| Volume | 23 |
| Nummer van het tijdschrift | 15 |
| DOI's | |
| Status | Gepubliceerd - 3 aug. 2022 |
Bibliografische nota
Publisher Copyright:© 2022 Wiley-VCH GmbH.
Financiering
Y. Su acknowledge the “Young Talent Support Plan” of Xi′an Jiaotong University and the Open Funds of State Key Laboratory of Physical Chemistry of Solid Surfaces (Xiamen University No. 202018). Supercomputing facilities were provided by the Hefei Advanced Computing Center. Y. Su acknowledge the “Young Talent Support Plan” of Xi′an Jiaotong University and the Open Funds of State Key Laboratory of Physical Chemistry of Solid Surfaces (Xiamen University No. 202018). Supercomputing facilities were provided by the Hefei Advanced Computing Center.