期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 59, 期 49, 页码 21904-21908出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202008785
关键词
electrocatalysis; magnetite single crystals; operando X-ray surface diffraction; oxide surface structures
资金
- AGENCIA [PICT 20141415, 2016069]
- EC-MEC [ANR-15-CE30-0024-01, DFG-Ma1618/2020]
- European Research Council-European Union's Horizon 2020 [864628]
- Austrian Science Fund FWF [Z-250]
- RyC program [RYC-2017-21931]
- Basque Government [IT-1255-19]
- ESRF
- European Research Council (ERC) [864628] Funding Source: European Research Council (ERC)
Establishing the atomic-scale structure of metal-oxide surfaces during electrochemical reactions is a key step to modeling this important class of electrocatalysts. Here, we demonstrate that the characteristic (root 2x root 2)R45 degrees surface reconstruction formed on (001)-oriented magnetite single crystals is maintained after immersion in 0.1 M NaOH at 0.20 V vs. Ag/AgCl and we investigate its dependence on the electrode potential. We follow the evolution of the surface using in situ and operando surface X-ray diffraction from the onset of hydrogen evolution, to potentials deep in the oxygen evolution reaction (OER) regime. The reconstruction remains stable for hours between -0.20 and 0.60 V and, surprisingly, is still present at anodic current densities of up to 10 mA cm(-2)and strongly affects the OER kinetics. We attribute this to a stabilization of the Fe(3)O(4)bulk by the reconstructed surface. At more negative potentials, a gradual and largely irreversible lifting of the reconstruction is observed due to the onset of oxide reduction.
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