Ferredoxin-Inspired Design of S-Synergized Fe-Fe Dual-Metal Center Catalysts for Enhanced Electrocatalytic Oxygen Reduction Reaction
© 2024 Wiley‐VCH GmbH.
| Veröffentlicht in: | Advanced materials (Deerfield Beach, Fla.). - 1998. - 36(2024), 19 vom: 09. Mai, Seite e2309231 |
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| 1. Verfasser: | |
| Weitere Verfasser: | , , , , , |
| Format: | Online-Aufsatz |
| Sprache: | English |
| Veröffentlicht: |
2024
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| Zugriff auf das übergeordnete Werk: | Advanced materials (Deerfield Beach, Fla.) |
| Schlagworte: | Journal Article dual‐metal center catalysts electronic modulation ferredoxin metal–organic framework oxygen reduction reaction |
| Zusammenfassung: | © 2024 Wiley‐VCH GmbH. Dual-metal center catalysts (DMCs) have shown the ability to enhance the oxygen reduction reaction (ORR) owing to their distinctive structural configurations. However, the precise modulation of electronic structure and the in-depth understanding of synergistic mechanisms between dual metal sites of DMCs at the atomic level remain challenging. Herein, mimicking the ferredoxin, Fe-based DMCs (Fe2N6-S) are strategically designed and fabricated, in which additional Fe and S sites are synchronously installed near the Fe sites and serve as "dual modulators" for coarse- and fine-tuning of the electronic modulation, respectively. The as-prepared Fe2N6-S catalyst exhibits enhanced ORR activity and outstanding Zinc-air (Zn-air) battery performance compared to the conventional single Fe site catalysts. The theoretical and experimental results reveal that introducing the second metal Fe creates a dual adsorption site that alters the O2 adsorption configuration and effectively activates the O─O bond, while the synergistic effect of dual Fe sites results in the downward shift of the d-band center, facilitating the release of OH*. Additionally, local electronic engineering of heteroatom S for Fe sites further facilitates the formation of the rate-determining step OOH*, thus accelerating the reaction kinetics |
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| Beschreibung: | Date Revised 09.05.2024 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
| ISSN: | 1521-4095 |
| DOI: | 10.1002/adma.202309231 |