Molecular Origin and Electrochemical Influence of Capacitive Surface States on Iron Oxide Photoanodes
The origin, the nature, and the electronic structure of surface defects causing surface states on metal oxides and their role in solar water splitting have been under scrutiny for several decades. In the present study, the surface of hematite films is treated with an oxygen plasma and then subject t...
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| Published in | Journal of physical chemistry. C Vol. 120; no. 6; pp. 3250 - 3258 |
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| Main Authors | , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
American Chemical Society
18.02.2016
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| Subjects | |
| Online Access | Get full text |
| ISSN | 1932-7447 1932-7455 1932-7455 |
| DOI | 10.1021/acs.jpcc.5b08013 |
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| Abstract | The origin, the nature, and the electronic structure of surface defects causing surface states on metal oxides and their role in solar water splitting have been under scrutiny for several decades. In the present study, the surface of hematite films is treated with an oxygen plasma and then subject to a detailed investigation with electroanalytical methods and element orbital specific X-ray spectroscopy. We observe a systemic variation of photoelectrochemical properties with oxygen treatment time. Fe 2p and O 1s core level X-ray photoelectron spectra and resonant valence band photoemission at the Fe 3p edge reveal the filling of prevalent oxygen vacancies with concomitant oxidation of Fe2+ to Fe3+ upon the oxygen treatment. The dc bias dependent impedance spectra confirm how a prevalent capacitive surface state, which evolves parallel with the photocurrent onset potential, becomes diminished upon oxygen treatment. Surface states of iron induce higher reactivity toward water oxidation than oxygen surface states. The correlation between oxygen vacancy filling, concentration of surface states, and photocurrent density in the course of treatment confirms that the surface defects are of a capacitive nature and that the onset of water splitting can be considered as a result of dielectric breakdown in an interfacial hydroxide layer between photoanode and water. |
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| AbstractList | The origin, the nature, and the electronic structure of surface defects causing surface states on metal oxides and their role in solar water splitting have been under scrutiny for several decades. In the present study, the surface of hematite films is treated with an oxygen plasma and then subject to a detailed investigation with electroanalytical methods and element orbital specific X-ray spectroscopy. We observe a systemic variation of photoelectrochemical properties with oxygen treatment time. Fe 2p and O 1s core level X-ray photoelectron spectra and resonant valence band photoemission at the Fe 3p edge reveal the filling of prevalent oxygen vacancies with concomitant oxidation of Fe2+ to Fe3+ upon the oxygen treatment. The dc bias dependent impedance spectra confirm how a prevalent capacitive surface state, which evolves parallel with the photocurrent onset potential, becomes diminished upon oxygen treatment. Surface states of iron induce higher reactivity toward water oxidation than oxygen surface states. The correlation between oxygen vacancy filling, concentration of surface states, and photocurrent density in the course of treatment confirms that the surface defects are of a capacitive nature and that the onset of water splitting can be considered as a result of dielectric breakdown in an interfacial hydroxide layer between photoanode and water. The origin, the nature, and the electronic structure of surface defects causing surface states on metal oxides and their role in solar water splitting have been under scrutiny for several decades. In the present study, the surface of hematite films is treated with an oxygen plasma and then subject to a detailed investigation with electroanalytical methods and element orbital specific X-ray spectroscopy. We observe a systemic variation of photoelectrochemical properties with oxygen treatment time. Fe 2p and O 1s core level X-ray photoelectron spectra and resonant valence band photoemission at the Fe 3p edge reveal the filling of prevalent oxygen vacancies with concomitant oxidation of Fe²⁺ to Fe³⁺ upon the oxygen treatment. The dc bias dependent impedance spectra confirm how a prevalent capacitive surface state, which evolves parallel with the photocurrent onset potential, becomes diminished upon oxygen treatment. Surface states of iron induce higher reactivity toward water oxidation than oxygen surface states. The correlation between oxygen vacancy filling, concentration of surface states, and photocurrent density in the course of treatment confirms that the surface defects are of a capacitive nature and that the onset of water splitting can be considered as a result of dielectric breakdown in an interfacial hydroxide layer between photoanode and water. |
| Author | Tsekouras, George Braun, Artur Bogdanoff, Peter Hermann-Geppert, Iris Boudoire, Florent Mun, Bongjin Simon Fortunato, Giuseppino Graetzel, Michael Hu, Yelin |
| AuthorAffiliation | Institute for Materials Technology University of Basel Laboratory of Photonics and Interfaces, Institute of Chemical Sciences and Engineering Helmholtz-Zentrum Geesthacht Gwangju Institute of Science and Technology Department of Chemistry Department of Physics and Photon Science, Ertl Center for Electrochemistry and Catalysis Protection and Physiology, Empa Helmut-Schmidt University Swiss Federal Laboratories for Materials Science and Technology Helmholtz-Zentrum Berlin für Materialien und Energie Institute for Materials Research, Sustainable Energy Technology Swiss Federal Institute of Technology Institute for Solar Fuels Laboratory for High Performance Ceramics, Empa |
| AuthorAffiliation_xml | – name: Swiss Federal Institute of Technology – name: Department of Chemistry – name: Laboratory of Photonics and Interfaces, Institute of Chemical Sciences and Engineering – name: Helmut-Schmidt University – name: Institute for Materials Technology – name: Helmholtz-Zentrum Geesthacht – name: Gwangju Institute of Science and Technology – name: Swiss Federal Laboratories for Materials Science and Technology – name: Laboratory for High Performance Ceramics, Empa – name: Protection and Physiology, Empa – name: Institute for Solar Fuels – name: University of Basel – name: Institute for Materials Research, Sustainable Energy Technology – name: Helmholtz-Zentrum Berlin für Materialien und Energie – name: Department of Physics and Photon Science, Ertl Center for Electrochemistry and Catalysis |
| Author_xml | – sequence: 1 givenname: Yelin surname: Hu fullname: Hu, Yelin – sequence: 2 givenname: Florent surname: Boudoire fullname: Boudoire, Florent – sequence: 3 givenname: Iris surname: Hermann-Geppert fullname: Hermann-Geppert, Iris – sequence: 4 givenname: Peter surname: Bogdanoff fullname: Bogdanoff, Peter – sequence: 5 givenname: George surname: Tsekouras fullname: Tsekouras, George – sequence: 6 givenname: Bongjin Simon surname: Mun fullname: Mun, Bongjin Simon – sequence: 7 givenname: Giuseppino surname: Fortunato fullname: Fortunato, Giuseppino – sequence: 8 givenname: Michael surname: Graetzel fullname: Graetzel, Michael – sequence: 9 givenname: Artur surname: Braun fullname: Braun, Artur email: artur.braun@alumni.ethz.ch |
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| SubjectTerms | electric current electrochemistry hematite iron oxidation oxygen physical chemistry X-radiation X-ray photoelectron spectroscopy |
| Title | Molecular Origin and Electrochemical Influence of Capacitive Surface States on Iron Oxide Photoanodes |
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