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| DOI | Trouver le DOI : https://doi.org/10.1038/s41467-024-45096-3 |
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| Auteur | Rechercher : Abdellah, Ahmed M.; Rechercher : Ismail, Fatma; Rechercher : Siig, Oliver W.Identifiant ORCID : https://orcid.org/0000-0003-4661-4721; Rechercher : Yang, Jie; Rechercher : Andrei, Carmen M.; Rechercher : DiCecco, Liza-Anastasia; Rechercher : Rakhsha, Amirhossein; Rechercher : Salem, Kholoud E.; Rechercher : Grandfield, KathrynIdentifiant ORCID : https://orcid.org/0000-0002-0188-9580; Rechercher : Bassim, NabilIdentifiant ORCID : https://orcid.org/0000-0002-9161-5769; Rechercher : Black, Robert1; Rechercher : Kastlunger, GeorgIdentifiant ORCID : https://orcid.org/0000-0002-3767-8734; Rechercher : Soleymani, LeylaIdentifiant ORCID : https://orcid.org/0000-0003-4915-2999; Rechercher : Higgins, DrewIdentifiant ORCID : https://orcid.org/0000-0002-0585-2670 |
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| Affiliation | - Conseil national de recherches Canada. Innovations dans les énergies propres
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| Format | Texte, Article |
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| Résumé | Electrochemical conversion of CO₂ offers a sustainable route for producing fuels and chemicals. Pd-based catalysts are effective for converting CO₂ into formate at low overpotentials and CO/H₂ at high overpotentials, while undergoing poorly understood morphology and phase structure transformations under reaction conditions that impact performance. Herein, in-situ liquid-phase transmission electron microscopy and select area diffraction measurements are applied to track the morphology and Pd/PdHₓ phase interconversion under reaction conditions as a function of electrode potential. These studies identify the degradation mechanisms, including poisoning and physical structure changes, occurring in PdHₓ/Pd electrodes. Constant potential density functional theory calculations are used to probe the reaction mechanisms occurring on the PdHₓ structures observed under reaction conditions. Microkinetic modeling reveals that the intercalation of *H into Pd is essential for formate production. However, the change in electrochemical CO₂ conversion selectivity away from formate and towards CO/H₂ at increasing overpotentials is due to electrode potential dependent changes in the reaction energetics and not a consequence of morphology or phase structure changes. |
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| Date de publication | 2023-01-31 |
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| Maison d’édition | Nature Research |
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| Licence | |
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| Dans | |
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| Note | Vidéos supplémentaires disponibles sur le site de l'éditeur |
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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 | 8e21e3a0-8a5d-412d-8bac-0cb07f5caca9 |
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| Enregistrement créé | 2024-04-11 |
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| Enregistrement modifié | 2024-04-17 |
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