Carbidisation of Pd nanoparticles by ethene decomposition, with methane production

Jones, Wilm, Wells, Peter P., Gibson, Emma K. , Chutia, Arunabhiram, Silverwood, Ian P., Catlow, C. Richard A. and Bowker, Michael (2019) Carbidisation of Pd nanoparticles by ethene decomposition, with methane production. ChemCatChem, 11 (17). pp. 4334-4339. ISSN 1867-3880

Full content URL: https://doi.org/10.1002/cctc.201900795

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Carbidisation of Pd nanoparticles by ethene decomposition, with methane production
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Abstract

In the presence of oxygenated organic molecules pure Pd, which is widely used in chemicals processing and the pharmaceutical industry, tends to defunctionalise and dehydrogenate such molecules to H2, CO and surface/bulk carbon, in the form of a palladium carbide. We have investigated the formation of this carbide by ethene adsorption using a variety of techniques, including pulsed flow reaction measurements, XAS and DFT calculations of the lattice expansion during carbidisation. These experiments show that two main reactions take place above 500K, that is, both total dehydrogenation, but also disproportionation to methane and the carbide, after which the activity of the Pd is completely lost. We estimate the value of x in PdCx to be 0.28 (±0.03), and show by computer modelling that this fits the lattice expansion observed by XAFS, and that there is charge transfer to C from Pd of around 0.2-0.4 e.

Keywords:Catalysis, Dehydrogenation, Disproportionation, Ethene, EXAFS, Palladium, Palladium Carbide, XAS, DFT
Subjects:F Physical Sciences > F100 Chemistry
Divisions:College of Science > School of Chemistry
ID Code:36271
Deposited On:23 Jul 2019 10:12

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