Biphase Pd Nanosheets with Atomic-Hybrid RhOx/Pd Amorphous Skins Disentangle the Activity-Stability Trade-Off in Oxygen Reduction Reaction
© 2024 Wiley‐VCH GmbH.
| Publié dans: | Advanced materials (Deerfield Beach, Fla.). - 1998. - 36(2024), 24 vom: 05. Juni, Seite e2314252 |
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| Auteur principal: | |
| Autres auteurs: | , , , , , , , , |
| Format: | Article en ligne |
| Langue: | English |
| Publié: |
2024
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| Accès à la collection: | Advanced materials (Deerfield Beach, Fla.) |
| Sujets: | Journal Article Pd‐based electrocatalysts RhOx/Pd interfaces activity‐stability trade‐off amorphous skins oxygen reduction reaction |
| Résumé: | © 2024 Wiley‐VCH GmbH. The activity-stability trade-off relationship of oxygen reduction reaction (ORR) is a tricky issue that strikes the electrocatalyst population and hinders the widespread application of fuel cells. Here neoteric biphase Pd nanosheets that are structured with ultrathin two-dimensional crystalline Pd inner cores and ≈1 nm thin atomic-hybrid RhOx/Pd amorphous skins, named c/a-PdPdRh NSs, for disentangling this trade-off dilemma for alkaline ORR are developed. The superthin amorphous skins significantly amplify the quantity of flexibly low-coordinated atoms for electrocatalysis. An in situ selected oxidation of the top-surface Rh dopants creates atomically hybrid RhOx/Pd disorder surfaces. Detailed energy spectra and theoretical simulation confirm that these RhOx/Pd interfaces can arouse a surface charge redistribution, causing significant electron deficiency and lowered d-band center for surface Pd. Meanwhile, anticorrosive Rh/RhOx species can thermodynamically passivate the neighboring Pd atoms from oxidative dissolution. Thanks to these amplified interfacial effects, the biphase c/a-Pd@PdRh NSs simultaneously exhibit a superhigh ORR activity (5.92 A mg-1, 22.8 times that of Pt/C) and an outstanding long-lasting stability after 100k cycles of accelerated durability test, showcasing unprecedented electrocatalysts for breaking the activity-stability trade-off relationship of ORR. This work paves a bran-new strategy for designing high-performance electrocatalysts through creating modulated amorphous skins on low-dimensional nanomaterials |
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| Description: | Date Revised 13.06.2024 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
| ISSN: | 1521-4095 |
| DOI: | 10.1002/adma.202314252 |