Modulation of Phase Transition in Cobalt Selenide with Simultaneous Construction of Heterojunctions for Highly-Efficient Oxygen Electrocatalysis in Zinc-Air Battery
© 2023 Wiley-VCH GmbH.
| Veröffentlicht in: | Advanced materials (Deerfield Beach, Fla.). - 1998. - 36(2024), 8 vom: 03. Feb., Seite e2306844 |
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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 cubic pyrite-CoSe2 electronic structure heterostructures phase transition engineering structure-property correlation |
| Zusammenfassung: | © 2023 Wiley-VCH GmbH. Phase transformation of cobalt selenide (CoSe2 ) can effectively modulate its intrinsic electrocatalytic activity. However, enhancing electroconductivity and catalytic activity/stability of CoSe2 still remains challenging. Heterostructure engineering may be feasible to optimize interfacial properties to promote the kinetics of oxygen electrocatalysis on a CoSe2 -based catalyst. Herein, a heterostructure consisting of CoSe2 and cobalt nitride (CoN) embedded in a hollow carbon cage is designed via a simultaneous phase/interface engineering strategy. Notably, the phase transition of orthorhombic-CoSe2 to cubic-CoSe2 (c-CoSe2 ) accompanied by in situ CoN formation is realized to build the c-CoSe2 /CoN heterointerface, which exhibits excellent/highly stable activities for oxygen reduction/evolution reactions (ORR/OER). Notably, heterostructure can modulate the local coordination environment and increase Co-Se/N bond lengths. Theoretical calculations show that Co-site (c-CoSe2 ) with an electronic state near Fermi energy level is the main active site for ORR/OER.Energetical tailoring of the d-orbital electronic structure of the Co atom of c-CoSe2 in heterostructure by in situ CoN incorporation lowers thermodynamic barriers for ORR/OER. Attractively, a zinc-air battery with a c-CoSe2 -CoN cathode displays excellent cycling stability (250 h) and charge/discharge voltage loss (0.953/0.96 V). It highlights that heterointerface engineering provides an option for modulating the bifunctional activity of metal selenides with controlled phase transformation |
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| Beschreibung: | Date Revised 22.02.2024 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
| ISSN: | 1521-4095 |
| DOI: | 10.1002/adma.202306844 |