Highly Exposed Ultra-Small High-Entropy Sulfides with d-p Orbital Hybridization for Efficient Oxygen Evolution
© 2025 Wiley‐VCH GmbH.
| Publié dans: | Advanced materials (Deerfield Beach, Fla.). - 1998. - 37(2025), 33 vom: 25. Aug., Seite e2508610 |
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| Auteur principal: | |
| Autres auteurs: | , , , , , , |
| Format: | Article en ligne |
| Langue: | English |
| Publié: |
2025
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| Accès à la collection: | Advanced materials (Deerfield Beach, Fla.) |
| Sujets: | Journal Article high‐entropy alloys high‐entropy sulfides orbital hybridization oxygen evolution reaction size engineering |
| Résumé: | © 2025 Wiley‐VCH GmbH. Precise regulation of electronic structure and nanoscale geometry represents a transformative strategy for breaking the activity-stability trade-off in oxygen evolution electrocatalysts. Here, highly exposed ultra-small high-entropy sulfides (HES, 5.2 nm) confined in porous carbon nanofibers are designed. This structure involves a dual-engineering synergistic effect combining d-p orbital hybridization and nanoconfinement. X-ray absorption spectroscopy (XAS) and density functional theory (DFT) calculations reveal hybridization between transition metal 3d orbitals and sulfur 3p orbitals. This orbital interaction induces a d-band center shift toward the Fermi level and facilitates interfacial charge redistribution, endowing HES with superior electron-donating capability to accelerate proton-coupled electron transfer kinetics. Such electronic modulation significantly optimizes the adsorption of oxygen evolution reaction (OER) intermediates (*OH, *O, *OOH). Experimentally, the HES demonstrates exceptional OER performance, exhibiting a low overpotential of 200 mV at 10 mA cm-2 and remarkable durability with negligible current decay during 300 h operation across current densities ranging from 10 to 100 mA cm-2. This work establishes a dual optimization strategy leveraging orbital hybridization engineering and size engineering for advanced electrocatalyst design, providing a new design approach in energy conversion technologies |
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| Description: | Date Revised 21.08.2025 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
| ISSN: | 1521-4095 |
| DOI: | 10.1002/adma.202508610 |