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In situ time resolved studies of hydride and deuteride formation in Pd/C electrodes via energy dispersive X-ray absorption spectroscopy

In situ time resolved studies of hydride and deuteride formation in Pd/C electrodes via energy dispersive X-ray absorption spectroscopy
In situ time resolved studies of hydride and deuteride formation in Pd/C electrodes via energy dispersive X-ray absorption spectroscopy
The electrochemical formation of beta-hydride and beta-deuteride phases of a carbon supported palladium nanoparticle catalyst has been investigated using time resolved in situ energy dispersive X-ray absorption spectroscopy (EDE) and the simultaneously collected chronoamperometric data. For the beta-hydride formation the rate of the phase transition was found to be limited by the rate of diffusion of H through the bulk of the Pd particles, while for b-deuteride formation the interfacial reduction of D+ was found to contribute more significantly to the kinetics. The composition of the hydride and deuteride phases formed was determined using both the lattice parameters obtained by fitting the EDE data and from linear sweep voltammograms, the former giving compositions of PdH0.83 and PdD0.63, which are consistent with the b-hydride and deuteride phases. Hyperstoichiometric compositions were obtained from the linear sweep voltammograms and the excess attributed to H or D spill-over on to the carbon support or re-oxidation of H-2 or D-2 trapped in the porous structure of the catalyst electrode.
multiple-scattering calculations, carbon-supported palladium, hydrogen absorption, fine-structure, particles, platinum, exafs, discharge, catalysts, clusters
1463-9076
366-372
Rose, A.
44dd032a-db31-411c-a86b-142829cba58f
South, O.
47d11aa2-cbe5-437b-b628-922682e8b39d
Harvey, I.
a8dffa7c-7412-4861-a03d-11e41d8632d7
Diaz-Moreno, S.
57fde3cb-73fa-48df-b505-79341096a3f1
Owen, J R.
067986ea-f3f3-4a83-bc87-7387cc5ac85d
Russell, A.E.
b6b7c748-efc1-4d5d-8a7a-8e4b69396169
Rose, A.
44dd032a-db31-411c-a86b-142829cba58f
South, O.
47d11aa2-cbe5-437b-b628-922682e8b39d
Harvey, I.
a8dffa7c-7412-4861-a03d-11e41d8632d7
Diaz-Moreno, S.
57fde3cb-73fa-48df-b505-79341096a3f1
Owen, J R.
067986ea-f3f3-4a83-bc87-7387cc5ac85d
Russell, A.E.
b6b7c748-efc1-4d5d-8a7a-8e4b69396169

Rose, A., South, O., Harvey, I., Diaz-Moreno, S., Owen, J R. and Russell, A.E. (2005) In situ time resolved studies of hydride and deuteride formation in Pd/C electrodes via energy dispersive X-ray absorption spectroscopy. Physical Chemistry Chemical Physics, 7 (2), 366-372. (doi:10.1039/b412066c).

Record type: Article

Abstract

The electrochemical formation of beta-hydride and beta-deuteride phases of a carbon supported palladium nanoparticle catalyst has been investigated using time resolved in situ energy dispersive X-ray absorption spectroscopy (EDE) and the simultaneously collected chronoamperometric data. For the beta-hydride formation the rate of the phase transition was found to be limited by the rate of diffusion of H through the bulk of the Pd particles, while for b-deuteride formation the interfacial reduction of D+ was found to contribute more significantly to the kinetics. The composition of the hydride and deuteride phases formed was determined using both the lattice parameters obtained by fitting the EDE data and from linear sweep voltammograms, the former giving compositions of PdH0.83 and PdD0.63, which are consistent with the b-hydride and deuteride phases. Hyperstoichiometric compositions were obtained from the linear sweep voltammograms and the excess attributed to H or D spill-over on to the carbon support or re-oxidation of H-2 or D-2 trapped in the porous structure of the catalyst electrode.

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More information

Published date: 2005
Additional Information: PCCP
Keywords: multiple-scattering calculations, carbon-supported palladium, hydrogen absorption, fine-structure, particles, platinum, exafs, discharge, catalysts, clusters

Identifiers

Local EPrints ID: 20898
URI: http://eprints.soton.ac.uk/id/eprint/20898
ISSN: 1463-9076
PURE UUID: cf48f6a8-1c52-47fe-9ac7-9f6f2b711849
ORCID for J R. Owen: ORCID iD orcid.org/0000-0002-4938-3693
ORCID for A.E. Russell: ORCID iD orcid.org/0000-0002-8382-6443

Catalogue record

Date deposited: 02 Mar 2006
Last modified: 16 Mar 2024 02:59

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Contributors

Author: A. Rose
Author: O. South
Author: I. Harvey
Author: S. Diaz-Moreno
Author: J R. Owen ORCID iD
Author: A.E. Russell ORCID iD

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