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Carbidisation of Pd Nanoparticles by Ethene Decomposition with Methane Production

Jones, W; Wells, PP; Gibson, EK; Chutia, A; Silverwood, IP; Catlow, CRA; Bowker, M; (2019) Carbidisation of Pd Nanoparticles by Ethene Decomposition with Methane Production. ChemCatChem , 11 (17) pp. 4334-4339. 10.1002/cctc.201900795. Green open access

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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.

Type: Article
Title: Carbidisation of Pd Nanoparticles by Ethene Decomposition with Methane Production
Open access status: An open access version is available from UCL Discovery
DOI: 10.1002/cctc.201900795
Publisher version: https://doi.org/10.1002/cctc.201900795
Language: English
Additional information: This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery-pp.ucl.ac.uk/id/eprint/10112384
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