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. ORCID: https://orcid.org/0000-0002-1341-1541 and Bowker, Michael ORCID: https://orcid.org/0000-0001-5075-1089 2019. Carbidisation of Pd nanoparticles by ethene decomposition, with methane production. ChemCatChem 11 (17) , pp. 4334-4339. 10.1002/cctc.201900795

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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 500 K, 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.

Item Type:	Article
Date Type:	Publication
Status:	Published
Schools:	Chemistry Cardiff Catalysis Institute (CCI)
Publisher:	Wiley
ISSN:	1867-3880
Funders:	EPSRC
Date of First Compliant Deposit:	5 July 2019
Date of Acceptance:	11 June 2019
Last Modified:	07 May 2023 10:22
URI:	https://orca.cardiff.ac.uk/id/eprint/124023

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