Carbidisation of Pd nanoparticles by ethene decomposition with methane production
Carbidisation of Pd nanoparticles by ethene decomposition with methane production
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.
Dehydrogenation, Disproportionation, Ethene, EXAFS, Palladium Carbide
4334-4339
Jones, Wilm
14b97080-56bc-4e8b-835b-72ad31ac4bc4
Wells, Peter P.
bc4fdc2d-a490-41bf-86cc-400edecf2266
Gibson, Emma K.
738c74e4-ab68-42fe-bda8-9d4a43669b31
Chutia, Arunabhiram
fe207bfe-0a7e-4369-8e62-bfa575399f83
Silverwood, Ian P.
82866f8b-db54-4b52-ae0e-20ac70e21b9e
Catlow, C. Richard A.
50b88125-9415-4b37-9146-af6783e42510
Bowker, Michael
c9ab10a5-d144-4533-bf6d-2fa16b669565
5 September 2019
Jones, Wilm
14b97080-56bc-4e8b-835b-72ad31ac4bc4
Wells, Peter P.
bc4fdc2d-a490-41bf-86cc-400edecf2266
Gibson, Emma K.
738c74e4-ab68-42fe-bda8-9d4a43669b31
Chutia, Arunabhiram
fe207bfe-0a7e-4369-8e62-bfa575399f83
Silverwood, Ian P.
82866f8b-db54-4b52-ae0e-20ac70e21b9e
Catlow, C. Richard A.
50b88125-9415-4b37-9146-af6783e42510
Bowker, Michael
c9ab10a5-d144-4533-bf6d-2fa16b669565
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), .
(doi:10.1002/cctc.201900795).
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.
Text
Jones_et_al-2019-ChemCatChem
- Version of Record
More information
e-pub ahead of print date: 17 June 2019
Published date: 5 September 2019
Keywords:
Dehydrogenation, Disproportionation, Ethene, EXAFS, Palladium Carbide
Identifiers
Local EPrints ID: 435368
URI: http://eprints.soton.ac.uk/id/eprint/435368
ISSN: 1867-3880
PURE UUID: 5398a836-7473-4b3b-ab3d-58072656a6d9
Catalogue record
Date deposited: 01 Nov 2019 17:30
Last modified: 18 Mar 2024 03:02
Export record
Altmetrics
Contributors
Author:
Wilm Jones
Author:
Emma K. Gibson
Author:
Arunabhiram Chutia
Author:
Ian P. Silverwood
Author:
C. Richard A. Catlow
Author:
Michael Bowker
Download statistics
Downloads from ePrints over the past year. Other digital versions may also be available to download e.g. from the publisher's website.
View more statistics
