Journal article
Towards identifying the active sites on RuO2(110) in catalyzing oxygen evolution
Massachusetts Institute of Technology1
University of Copenhagen2
Surface Physics and Catalysis, Department of Physics, Technical University of Denmark3
Department of Energy Conversion and Storage, Technical University of Denmark4
Atomic Scale Materials Modelling, Department of Energy Conversion and Storage, Technical University of Denmark5
Computational Atomic-scale Materials Design, Department of Physics, Technical University of Denmark6
Department of Physics, Technical University of Denmark7
Neutrons and X-rays for Materials Physics, Department of Physics, Technical University of Denmark8
SLAC National Accelerator Laboratory9
Argonne National Laboratory10
Oregon State University11
...and 1 moreWhile the surface atomic structure of RuO2 has been well studied in ultra high vacuum, much less is known about the interaction between water and RuO2 in aqueous solution. In this work, in situ surface X-ray scattering measurements combined with density functional theory (DFT) were used to determine the surface structural changes on single-crystal RuO2(110) as a function of potential in acidic electrolyte.
The redox peaks at 0.7, 1.1 and 1.4 V vs. reversible hydrogen electrode (RHE) could be attributed to surface transitions associated with the successive deprotonation of –H2O on the coordinatively unsaturated Ru sites (CUS) and hydrogen adsorbed to the bridging oxygen sites. At potentials relevant to the oxygen evolution reaction (OER), an –OO species on the Ru CUS sites was detected, which was stabilized by a neighboring –OH group on the Ru CUS or bridge site.
Combining potential-dependent surface structures with their energetics from DFT led to a new OER pathway, where the deprotonation of the –OH group used to stabilize –OO was found to be rate-limiting.
Language: | English |
---|---|
Publisher: | The Royal Society of Chemistry |
Year: | 2017 |
Pages: | 2626-2637 |
ISSN: | 17545706 and 17545692 |
Types: | Journal article |
DOI: | 10.1039/c7ee02307c |
ORCIDs: | Pedersen, Anders Filsøe , Hansen, Heine Anton , Vegge, Tejs , Chorkendorff, Ib , Stephens, Ifan , 0000-0002-6655-3105 , 0000-0003-2878-6976 , 0000-0001-7598-5076 , 0000-0001-8714-2121 and 0000-0001-7749-6567 |