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Title: New insights into water splitting at mesoporous alpha-Fe2O3 films: a study by modulated transmittance and impedance spectroscopies
Authors: Cummings, Charles Y.
Marken, Frank
Peter, Laurence M.
Wijayantha, K.G.U.
Tahir, Asif A.
Issue Date: 2012
Publisher: © American Chemical Society
Citation: CUMMINGS, C.Y. ... et al., 2012. New insights into water splitting at mesoporous alpha-Fe2O3 films: a study by modulated transmittance and impedance spectroscopies. Journal of the American Chemical Society, 134 (2), pp. 1228 - 1234.
Abstract: Thin mesoporous films of α-Fe2O3 have been prepared on conducting glass substrates using layer-by-layer self-assembly of ca. 4 nm hydrous oxide nanoparticles followed by calcining. The electrodes were used to study the oxygen evolution reaction (OER) in the dark and under illumination using in situ potential-modulated absorption spectroscopy (PMAS) and light-modulated absorption spectroscopy (LMAS) combined with impedance spectroscopy. Formation of surface-bound higher-valent iron species (or “surface trapped holes”) was deduced from the PMAS spectra measured in the OER onset region. Similar LMAS spectra were obtained at more negative potentials in the onset region of photoelectrochemical OER, indicating involvement of the same intermediates. The impedance response of the mesoporous α-Fe2O3 electrodes exhibits characteristic transmission line behavior that is attributed to slow hopping of holes, probably between surface iron species. Frequency-resolved PMAS and LMAS measurements revealed slow relaxation behavior that can be related to the impedance response and that indicates that the lifetime of the intermediates (or trapped holes) involved in the OER is remarkably long.
Description: Closed access. This article was published in the Journal of the American Chemical Society [© American Chemical Society] and the definitive version is available at: http://dx.doi.org/10.1021/ja209530s
Sponsor: K.G.U.W. and A.A.T. would like to acknowledge the support given by UK EPSRC
Version: Published
DOI: 10.1021/ja209530s
URI: https://dspace.lboro.ac.uk/2134/15778
Publisher Link: http://dx.doi.org/10.1021/ja209530s
ISSN: 0002-7863
Appears in Collections:Closed Access (Chemistry)

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