Dual Single-Atomic Ni-N4 and Fe-N4 Sites Constructing Janus Hollow Graphene for Selective Oxygen Electrocatalysis
© 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Veröffentlicht in: | Advanced materials (Deerfield Beach, Fla.). - 1998. - 32(2020), 30 vom: 22. Juli, Seite e2003134 |
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1. Verfasser: | |
Weitere Verfasser: | , , , , , , |
Format: | Online-Aufsatz |
Sprache: | English |
Veröffentlicht: |
2020
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Zugriff auf das übergeordnete Werk: | Advanced materials (Deerfield Beach, Fla.) |
Schlagworte: | Journal Article Janus catalysts Zn-air batteries bifunctional electrocatalysis single atoms |
Zusammenfassung: | © 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. Nitrogen-coordinated metal single atoms in carbon have aroused extensive interest recently and have been growing as an active research frontier in a wide range of key renewable energy reactions and devices. Herein, a step-by-step self-assembly strategy is developed to allocate nickel (Ni) and iron (Fe) single atoms respectively on the inner and outer walls of graphene hollow nanospheres (GHSs), realizing separate-sided different single-atom functionalization of hollow graphene. The Ni or Fe single atom is demonstrated to be coordinated with four N atoms via the formation of a Ni-N4 or Fe-N4 planar configuration. The developed Ni-N4 /GHSs/Fe-N4 Janus material exhibits excellent bifunctional electrocatalytic performance, in which the outer Fe-N4 clusters dominantly contribute to high activity toward the oxygen reduction reaction (ORR), while the inner Ni-N4 clusters are responsible for excellent activity toward the oxygen evolution reaction (OER). Density functional theory calculations demonstrate the structures and reactivities of Fe-N4 and Ni-N4 for the ORR and OER. The Ni-N4 /GHSs/Fe-N4 endows a rechargeable Zn-air battery with excellent energy efficiency and cycling stability as an air-cathode, outperforming that of the benchmark Pt/C+RuO2 air-cathode. The current work paves a new avenue for precise control of single-atom sites on carbon surface for the high-performance and selective electrocatalysts |
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Beschreibung: | Date Revised 16.11.2020 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
ISSN: | 1521-4095 |
DOI: | 10.1002/adma.202003134 |