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Structural changes of highly active Pd/MeOx (Me = Fe, Co, Ni) during catalytic methane combustion
- Fe2O3, Co3O4 and NiO nanoparticles were prepared via a citrate method and further functionalized with Pd by impregnation. The pure oxides as well as Pd/Fe2O3, Pd/Co3O4, and Pd/NiO (1, 5 and 10 wt % Pd) were employed for catalytic methane combustion under methane lean (1 vol %)/oxygen rich (18 vol %, balanced with nitrogen) conditions. Already, the pure metal oxides showed a high catalytic activity leading to complete conversion temperature of T100 ≤ 500 °C. H2-TPR (Temperature-programmed reduction) experiments revealed that Pd-functionalized metal oxides exhibited enhanced redox activity compared to the pure oxides leading to improved catalytic combustion activity at lower temperatures. At a loading of 1 wt % Pd, 1Pd/Co3O4 (T100 = 360 °C) outperforms 1Pd/Fe2O3 (T100 = 410 °C) as well as 1Pd/NiO (T100 = 380 °C). At a loading of 10 wt % Pd, T100 could only be slightly reduced in all cases. 1Pd/Co3O4 and 1Pd/NiO show reasonable stability over 70 h on stream at T100. XPS (X-rayFe2O3, Co3O4 and NiO nanoparticles were prepared via a citrate method and further functionalized with Pd by impregnation. The pure oxides as well as Pd/Fe2O3, Pd/Co3O4, and Pd/NiO (1, 5 and 10 wt % Pd) were employed for catalytic methane combustion under methane lean (1 vol %)/oxygen rich (18 vol %, balanced with nitrogen) conditions. Already, the pure metal oxides showed a high catalytic activity leading to complete conversion temperature of T100 ≤ 500 °C. H2-TPR (Temperature-programmed reduction) experiments revealed that Pd-functionalized metal oxides exhibited enhanced redox activity compared to the pure oxides leading to improved catalytic combustion activity at lower temperatures. At a loading of 1 wt % Pd, 1Pd/Co3O4 (T100 = 360 °C) outperforms 1Pd/Fe2O3 (T100 = 410 °C) as well as 1Pd/NiO (T100 = 380 °C). At a loading of 10 wt % Pd, T100 could only be slightly reduced in all cases. 1Pd/Co3O4 and 1Pd/NiO show reasonable stability over 70 h on stream at T100. XPS (X-ray photoelectron spectroscopy) and STEM (Scanning transmission electron microscopy) investigations revealed strong interactions between Pd and NiO as well as Co3O4, respectively, leading to dynamic transformations and reoxidation of Pd due to solid state reactions, which leads to the high long-term stability.…
Autor*innen: | Dominik Seeburg, Dongjing Liu, Jörg RadnikORCiD, Hanan Atia, Marga-Martina Pohl, Matthias Schneider, Andreas Martin, Sebastian Wohlrab |
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Dokumenttyp: | Zeitschriftenartikel |
Veröffentlichungsform: | Verlagsliteratur |
Sprache: | Englisch |
Titel des übergeordneten Werkes (Englisch): | Catalysts |
Jahr der Erstveröffentlichung: | 2018 |
Organisationseinheit der BAM: | 6 Materialchemie |
6 Materialchemie / 6.1 Oberflächen- und Dünnschichtanalyse | |
Veröffentlichende Institution: | Bundesanstalt für Materialforschung und -prüfung (BAM) |
Verlag: | MDPI |
Jahrgang/Band: | 8 |
Ausgabe/Heft: | 2 |
Erste Seite: | Article 42, 1 |
Letzte Seite: | 13 |
DDC-Klassifikation: | Naturwissenschaften und Mathematik / Chemie / Analytische Chemie |
Freie Schlagwörter: | Carbon dioxide; Methane removal; Methane total oxidation; X-ray photoelectron spectroscopy |
Themenfelder/Aktivitätsfelder der BAM: | Chemie und Prozesstechnik |
DOI: | 10.3390/catal8020042 |
URN: | urn:nbn:de:kobv:b43-439412 |
ISSN: | 2073-4344 |
Verfügbarkeit des Dokuments: | Datei für die Öffentlichkeit verfügbar ("Open Access") |
Lizenz (Deutsch): | Creative Commons - CC BY - Namensnennung 4.0 International |
Datum der Freischaltung: | 30.01.2018 |
Referierte Publikation: | Ja |
Datum der Eintragung als referierte Publikation: | 09.04.2018 |
Schriftenreihen ohne Nummerierung: | Wissenschaftliche Artikel der BAM |