Electronically and Geometrically Modified Single-Atom Fe Sites by Adjacent Fe Nanoparticles for Enhanced Oxygen Reduction
© 2021 Wiley-VCH GmbH.
| Veröffentlicht in: | Advanced materials (Deerfield Beach, Fla.). - 1998. - 34(2022), 5 vom: 15. Feb., Seite e2107291 |
|---|---|
| 1. Verfasser: | |
| Weitere Verfasser: | , , , |
| Format: | Online-Aufsatz |
| Sprache: | English |
| Veröffentlicht: |
2022
|
| Zugriff auf das übergeordnete Werk: | Advanced materials (Deerfield Beach, Fla.) |
| Schlagworte: | Journal Article Fe nanoparticles atomic FeN(O)x sites electronic modification geometric modification oxygen reduction reaction |
| Zusammenfassung: | © 2021 Wiley-VCH GmbH. Fe-N-C materials exhibit excellent activity and stability for oxygen reduction reaction (ORR), as one of the most promising candidates to replace commercial Pt/C catalysts. However, it is challenging to unravel features of the superior ORR activity originating from Fe-N-C materials. In this work, the electronic and geometric structures of the isolated Fe-N-C sites and their correlations with the ORR performance are investigated by varying the secondary thermal activation temperature of a rationally designed NC-supported Fe single-atom catalyst (SAC). The systematic analyses demonstrate the significant role of coordinated atoms of SA and metallic Fe nanoparticles (NPs) in altering the electronic structure of isolated Fe-N-C sites. Meanwhile, strong interaction between isolated Fe-N-C sites and adjacent Fe NPs can change the geometric structure of isolated Fe-N-C sites. Theoretical calculations reveal that optimal regulation of the electronic and geometric structure of isolated Fe-N-C sites by the co-existence of Fe NPs narrows the energy barriers of the rate-limiting steps of ORR, resulting in outstanding ORR performance. This work not only provides the fundamental understanding of the underlying structure-activity relationship, but also sheds light on designing efficient Fe-N-C catalysts |
|---|---|
| Beschreibung: | Date Revised 03.02.2022 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
| ISSN: | 1521-4095 |
| DOI: | 10.1002/adma.202107291 |