Wörz, Nicolai ; Brandner, Armin ; Claus, Peter (2010)
Platinum-Bismuth Catalyzed Oxidation of Glycerol: Kinetics and the Origin of Selective Deactivation.
In: The Journal of Physical Chemistry C, 114 (2)
doi: 10.1021/jp909412h
Artikel, Bibliographie
Kurzbeschreibung (Abstract)
The selective oxidation of glycerol to dihydroxyacetone is still a challenging task for heterogeneous catalysis and important to the chemical industry. Especially bimetallic Pt−Bi catalysts show a high initial selectivity to dihydroxyacetone in acidic media but exhibit a strong deactivation during reaction as well. This deactivation decreases activity as well as selectivity to dihydroxyacetone. Thus, only moderate yields may be achieved. In this work, product adsorption was identified as a major cause. In particular, glyceric acid, an oxidation product of the primary hydroxyl group, selectively blocks those kinds of active sites that are predominantly responsible for dihydroxyacetone formation. This could be confirmed by means of kinetic modeling. It has been proven that all catalytic experiments taken into account for the parameter estimation are free from external and internal transport limitations. A mechanism characterized by two different active sites has been derived. Glyceric acid selectively inhibits one of them, causing the observed decrease in dihydroxyacetone selectivity and catalyst activity.
| Typ des Eintrags: | Artikel |
|---|---|
| Erschienen: | 2010 |
| Autor(en): | Wörz, Nicolai ; Brandner, Armin ; Claus, Peter |
| Art des Eintrags: | Bibliographie |
| Titel: | Platinum-Bismuth Catalyzed Oxidation of Glycerol: Kinetics and the Origin of Selective Deactivation |
| Sprache: | Englisch |
| Publikationsjahr: | 21 Januar 2010 |
| Titel der Zeitschrift, Zeitung oder Schriftenreihe: | The Journal of Physical Chemistry C |
| Jahrgang/Volume einer Zeitschrift: | 114 |
| (Heft-)Nummer: | 2 |
| DOI: | 10.1021/jp909412h |
| Kurzbeschreibung (Abstract): | The selective oxidation of glycerol to dihydroxyacetone is still a challenging task for heterogeneous catalysis and important to the chemical industry. Especially bimetallic Pt−Bi catalysts show a high initial selectivity to dihydroxyacetone in acidic media but exhibit a strong deactivation during reaction as well. This deactivation decreases activity as well as selectivity to dihydroxyacetone. Thus, only moderate yields may be achieved. In this work, product adsorption was identified as a major cause. In particular, glyceric acid, an oxidation product of the primary hydroxyl group, selectively blocks those kinds of active sites that are predominantly responsible for dihydroxyacetone formation. This could be confirmed by means of kinetic modeling. It has been proven that all catalytic experiments taken into account for the parameter estimation are free from external and internal transport limitations. A mechanism characterized by two different active sites has been derived. Glyceric acid selectively inhibits one of them, causing the observed decrease in dihydroxyacetone selectivity and catalyst activity. |
| Zusätzliche Informationen: | Publication Date (Web): 9. Dezember 2009 |
| Fachbereich(e)/-gebiet(e): | 07 Fachbereich Chemie 07 Fachbereich Chemie > Ernst-Berl-Institut > Fachgebiet Technische Chemie > Technische Chemie II 07 Fachbereich Chemie > Ernst-Berl-Institut > Fachgebiet Technische Chemie |
| Hinterlegungsdatum: | 16 Nov 2009 09:57 |
| Letzte Änderung: | 05 Mär 2013 09:27 |
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