Atomically Dispersed Co2 MnN8 Triatomic Sites Anchored in N-Doped Carbon Enabling Efficient Oxygen Reduction Reaction
© 2023 Wiley-VCH GmbH.
Veröffentlicht in: | Advanced materials (Deerfield Beach, Fla.). - 1998. - 35(2023), 42 vom: 05. Okt., Seite e2210975 |
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1. Verfasser: | |
Weitere Verfasser: | , , , , , , , , |
Format: | Online-Aufsatz |
Sprache: | English |
Veröffentlicht: |
2023
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Zugriff auf das übergeordnete Werk: | Advanced materials (Deerfield Beach, Fla.) |
Schlagworte: | Journal Article Co2MnN8 electrocatalysts half-filled oxygen reduction reaction trinuclear structures |
Zusammenfassung: | © 2023 Wiley-VCH GmbH. Atomically dispersed transition metal-nitrogen/carbon (M-N/C) catalysts have emerged as the most promising substitutes to the precious platinum counterparts toward the oxygen reduction reaction (ORR). However, the reported M-N/C catalysts are usually in the form of common M-N4 moieties with only a single metal active site, and they suffer from insufficient activity. Herein, an unusual trinuclear active structure is elaborately developed with a nitrogen-coordinated single Mn atom adjacent to two Co atoms (Co2 MnN8 ) anchored in N-doped carbon as a highly efficient ORR catalyst via adsorption-pyrolysis of a bimetallic zeolitic imidazolate framework precursor. Atomic structural investigations and density functional theory (DFT) calculations reveal that Co2 MnN8 would experience a spontaneous OH binding to form Co2 MnN8 -2OH as the real active site, leading to a single electron-filled state in the d z 2 ${\mathrm{d}}_{{z}^{2}}$ orbital and an optimized binding energy of intermediates. Accordingly, the as-developed Co2 MnN8 /C exhibits an unprecedented ORR activity with a high half-wave potential of 0.912 V and outstanding stability, not only surpassing the Pt/C catalyst but also representing a new record for the Co-based catalyst |
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Beschreibung: | Date Revised 20.10.2023 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
ISSN: | 1521-4095 |
DOI: | 10.1002/adma.202210975 |