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| DOI | Trouver le DOI : https://doi.org/10.1021/acsami.4c01105 |
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| Auteur | Rechercher : Whittingham, Alexander W. H.1Identifiant ORCID : https://orcid.org/0000-0001-9752-6356; Rechercher : Boke, Marlyn; Rechercher : Smith, Rodney D. L.Identifiant ORCID : https://orcid.org/0000-0003-1209-9653 |
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| Affiliation | - Conseil national de recherches Canada. Innovations dans les énergies propres
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| Bailleur de fonds | Rechercher : Ontario Research Foundation; Rechercher : Natural Sciences and Engineering Research Council of Canada |
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| Format | Texte, Article |
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| Sujet | perovskite; oxygen reduction reaction; reaction mechanism; electrocatalysis; peroxide production; lattice distortions |
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| Résumé | Compositional tuning of layered perovskite oxidesprovides a means of systematically studying how local distortionsaffect fundamental aspects of electrochemical reaction pathways.Structural analysis of a family of samples La₁.₂Sr₀.₈Ni₁₋yCoyO₄ showsthat Ni-rich compositions have an expanded crystalline c axis, which isanisotropically compressed by systematic Co incorporation. Ramanspectra reveal the strong growth of a symmetry forbidden mode,which suggests that Co acts through localized distortions. Crystallo-graphic and spectroscopic parameters describing this structuraldistortion correlate to the measured Tafel slopes for the oxygenreduction reaction for all Ni-containing samples, which is attributedto the distortion of potential energy surfaces by the Jahn−Tellerexpansion of d⁷ Ni(III) cations. Incorporation of Co not only minimizes the distortion but alters the apparent selectivity of theoxygen reduction reaction away from H₂O₂ and toward H₂O. Rotating ring-disk electrochemical measurements, however, indicatethat the apparent change in selectivity is due to activation of a first-order chemical disproportionation of H₂O₂ that is activated byCo in the lattice. These outcomes will support efforts to design electrocatalysts and reactors for the electrochemical synthesis ofH₂O₂. |
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| Date de publication | 2024-04-11 |
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| Maison d’édition | American Chemical Society |
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| Dans | |
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| Langue | anglais |
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| Publications évaluées par des pairs | Oui |
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| Exporter la notice | Exporter en format RIS |
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| Signaler une correction | Signaler une correction (s'ouvre dans un nouvel onglet) |
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| Identificateur de l’enregistrement | ae1e497c-0118-4c5c-bbdd-46a02121b9a2 |
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| Enregistrement créé | 2024-05-15 |
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| Enregistrement modifié | 2025-11-06 |
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