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Different promoting roles of ruthenium for the oxidation of primary and secondary alcohols on PtRu electrocatalysts

  • This study shows remarkably different features between the oxidation of secondary and primary C₃-C₅ alcohols. The oxidation of primary alcohols is controlled by the oxidative removal of blocking adsorbates, such as CO, formed after the dissociative adsorption of alcohol molecules. Conversely, secondary alcohols do not undergo dissociative adsorption and therefore their oxidation is purely controlled by the energetics of the elementary reaction steps. In this respect, a different role of ruthenium is revealed for the electrooxidation of primary and secondary alcohols on bimetallic platinum-ruthenium catalysts. Ruthenium enhances the oxidation of primary alcohols via the established bifunctional mechanism, in which the adsorption of (hydr)oxide species that are necessary to remove the blocking adsorbates is favored. In contrast, the oxidation of secondary alcohols is enhanced by the Ru-assisted stabilization of an O-bound intermediate that is involved in the potential-limiting step. ThisThis study shows remarkably different features between the oxidation of secondary and primary C₃-C₅ alcohols. The oxidation of primary alcohols is controlled by the oxidative removal of blocking adsorbates, such as CO, formed after the dissociative adsorption of alcohol molecules. Conversely, secondary alcohols do not undergo dissociative adsorption and therefore their oxidation is purely controlled by the energetics of the elementary reaction steps. In this respect, a different role of ruthenium is revealed for the electrooxidation of primary and secondary alcohols on bimetallic platinum-ruthenium catalysts. Ruthenium enhances the oxidation of primary alcohols via the established bifunctional mechanism, in which the adsorption of (hydr)oxide species that are necessary to remove the blocking adsorbates is favored. In contrast, the oxidation of secondary alcohols is enhanced by the Ru-assisted stabilization of an O-bound intermediate that is involved in the potential-limiting step. This alternative pathway enables the oxidation of secondary alcohols close to the equilibrium potential.zeige mehrzeige weniger

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Metadaten
Autor*innen:I. Mangoufis-Giasin, O. Piqué, Peyman KhanipourORCiD, K. J. J. Mayrhofer, F. Calle-Vallejo, I. Katsounaros
Dokumenttyp:Zeitschriftenartikel
Veröffentlichungsform:Verlagsliteratur
Sprache:Englisch
Titel des übergeordneten Werkes (Englisch):Journal of catalysis
Jahr der Erstveröffentlichung:2021
Organisationseinheit der BAM:1 Analytische Chemie; Referenzmaterialien
1 Analytische Chemie; Referenzmaterialien / 1.4 Prozessanalytik
Verlag:Elsevier
Verlagsort:San Diego, Calif.
Jahrgang/Band:400
Erste Seite:166
Letzte Seite:172
DDC-Klassifikation:Naturwissenschaften und Mathematik / Chemie / Analytische Chemie
Freie Schlagwörter:2-propanol oxidation; Alcohol electrooxidation; Density functional theory; Direct alcohol fuel cells; Electrocatalysis; Electrochemical energy conversion; Electrochemical real-time mass spectrometry; Secondary alcohols
Themenfelder/Aktivitätsfelder der BAM:Chemie und Prozesstechnik
Chemie und Prozesstechnik / Chemische Charakterisierung und Spurenanalytik
DOI:10.1016/j.jcat.2021.05.028
ISSN:0021-9517
Verfügbarkeit des Dokuments:Datei im Netzwerk der BAM verfügbar ("Closed Access")
Datum der Freischaltung:14.02.2023
Referierte Publikation:Ja
Datum der Eintragung als referierte Publikation:14.02.2023
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