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The decarbonylation of acetaldehyde on Pd crystals and on supported catalysts

Bowker, Michael, Cookson, Lucinda Sarah, Bhantoo, Jenita Rhiannon, Carley, Albert Frederick, Hayden, Edward William, Gilbert, Lee Alexander, Morgan, Christian, Counsell, Jonathan David and Yaseneva, Polina 2011. The decarbonylation of acetaldehyde on Pd crystals and on supported catalysts. Applied Catalysis A: General 391 (1-2) , pp. 394-399. 10.1016/j.apcata.2010.05.012

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Abstract

The reaction of acetaldehyde with pure Pd (in single crystal form, Pd(1 1 0) and Pd(1 1 1)) and with nanoparticles of Pd supported on silica have been investigated. The main reactions involved are decarbonylation (to produce CO and methane) and dehydrogenation (to produce CO, H2 and carbon), and both of these reactions are seen on the unsupported and supported forms of Pd. In general the behaviour is similar, but there is a marked contrast in the temperature dependence of the reaction on single crystals and on the catalysts. On the crystals there is a sharp transition between decarbonylation and dehydrogenation, occurring at 420 K, whereas the catalysts show little activity for dehydrogenation, even up to 600 K. The reason for this relates to the capacity of the samples to absorb the carbon product of dehydrogenation into the bulk of the sample. The single crystal samples have a very low surface:bulk ratio and C formed at the surface is quickly lost to the bulk above 420 K, leaving an apparently clean and reactive Pd surface. The catalysts on the other hand, due to their high surface:bulk ratio, quickly become carbidised and are thereby passivated towards dehydrogenation, favouring high selectivity to decarbonylation. This proves that Pd catalysts are dehydrogenation catalysts and are only more selective to other routes when passivated by bulk carbon (or other additives such as Au).

Item Type: Article
Date Type: Publication
Status: Published
Schools: Chemistry
Cardiff Catalysis Institute (CCI)
Subjects: Q Science > QD Chemistry
Uncontrolled Keywords: Acetaldehyde decarbonylation; Palladium catalysts; Single crystal Pd; Surface carbon; Acetaldehyde dehydrogenation; Pulsed flow reactor; Molecular beam reactor
Publisher: Elsevier
ISSN: 0926-860X
Last Modified: 04 Jul 2019 21:15
URI: http://orca-mwe.cf.ac.uk/id/eprint/12419

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