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Carbidisation of Pd nanoparticles by ethene decomposition, with methane production

DOI: 10.1002/cctc.201900795 DOI Help

Authors: Michael Bowker (Cardiff University) , Wilm Jones (UK Catalysis Hub, Research Complex at Harwell) , Peter P. Wells (UK Catalysis Hub, Research Complex at Harwell; Diamond Light Source; University of Southampton) , Emma K. Gibson (UK Catalysis Hub, Research Complex at Harwell; University of Glasgow) , Arunabhiram Chutia (UK Catalysis Hub, Research Complex at Harwell; University of Lincoln) , Ian P. Silverwood (ISIS Neutron and Muon Facility) , C. Richard A. Catlow (UK Catalysis Hub, Research Complex at Harwell)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Chemcatchem

State: Published (Approved)
Published: June 2019

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.

Journal Keywords: Catalysis; Dehydrogenation; Disproportionation; Ethene; EXAFS; Palladium; Palladium Carbide; XAS

Subject Areas: Chemistry


Instruments: B18-Core EXAFS