Journal
CATALYSIS TODAY
Volume 260, Issue -, Pages 72-81Publisher
ELSEVIER SCIENCE BV
DOI: 10.1016/j.cattod.2015.07.024
Keywords
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Funding
- Swiss Federal Office of Energy [152316-101883, 153613-102809, 153476-102691]
- European Community [227179]
- Swiss NSF [206021-121306, 200021-132126, 200021-137868]
- Indo-Swiss project ISJRP [138 864]
- Swiss National Science Foundation (SNF) [200021_137868, 200021_132126] Funding Source: Swiss National Science Foundation (SNF)
- Directorate For Geosciences
- Division Of Earth Sciences [1148494] Funding Source: National Science Foundation
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We re-assess experimental soft X-ray absorption spectra of the oxygen K-shell which we recorded operando from iron oxide during photoelectrochemical water splitting in KOH electrolyte. In particular, we refer to recently reported transitional electron hole states which originate within the charge carrier depletion layer of the iron oxide and on the iron oxide surface. For the latter we find that an intermediate oxy-peroxo species is formed on the iron oxide with increasing bias potential, which disappears upon further polarization of the electrode, concomitantly with the evolution and disappearance of the aforementioned surface state. The oxygen spectra contain also the spectroscopic signatures of the electrolyte water, the position of which changes with increasing bias potential towards lower X-ray energies, revealing the breaking and formation of hydrogen bonds in the water during the experiment. Combined with potential dependent impedance spectroscopy data we are able to sketch the molecular structure of chemical intermediates and their charge carrier dynamics. (C) 2015 Elsevier B.V. All rights reserved.
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