Examining the Structure Sensitivity of the Oxygen Evolution Reaction on Pt Single-Crystal Electrodes: A Combined Experimental and Theoretical Study.
density functional theory
oxygen evolution reaction
platinum
single crystals
structure sensitivity
Journal
Chemphyschem : a European journal of chemical physics and physical chemistry
ISSN: 1439-7641
Titre abrégé: Chemphyschem
Pays: Germany
ID NLM: 100954211
Informations de publication
Date de publication:
19 11 2019
19 11 2019
Historique:
received:
29
01
2019
revised:
29
03
2019
pubmed:
3
4
2019
medline:
3
4
2019
entrez:
3
4
2019
Statut:
ppublish
Résumé
In the present work we investigate the structure sensitivity of the oxygen evolution reaction (OER) combining electrochemistry, in situ spectroscopy and density functional theory calculations. The intrinsic difficulty of such studies is the fact that at electrode potentials where the OER is observed, the electrode material is highly oxidized. As a consequence, the surface structure during the reaction is in general ill-defined and only scarce knowledge exists concerning the structure-activity relationship of this important reaction. To alleviate these challenging conditions, we chose as starting point well-defined Pt single-crystal electrodes, which we exposed to well-defined conditioning before studying their OER rate. Using this approach, a potential region is identified where the OER on Pt is indeed structure-sensitive with Pt(100) being significantly more active than Pt(111). This experimental finding is in contrast to a DFT analysis of the adsorption strength of the reaction intermediates O*, OH*, and OOH* often used to plot the activity in a volcano curve. It is proposed that as a consequence of the highly oxidizing conditions, the structure-sensitive charge-transfer resistance through the interface determines the observed reaction rate.
Identifiants
pubmed: 30938896
doi: 10.1002/cphc.201900193
doi:
Types de publication
Journal Article
Research Support, Non-U.S. Gov't
Langues
eng
Sous-ensembles de citation
IM
Pagination
3154-3162Subventions
Organisme : SNF Professorship
ID : PP00P2_157615
Pays : International
Organisme : UBELIX
Pays : International
Organisme : University of Bern
Pays : International
Informations de copyright
© 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.
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