Room temperature redox reaction by oxide ion migration at carbon/Gd-doped CeO2 heterointerface probed by an in situ hard x-ray photoemission and soft x-ray absorption spectroscopies

In situ hard x-ray photoemission spectroscopy (HX-PES) and soft x-ray absorption spectroscopy (SX-XAS) have been employed to investigate a local redox reaction at the carbon/Gd-doped CeO 2 (GDC) thin film heterointerface under applied dc bias. In HX-PES, Ce3d and O1s core levels show a parallel chem...

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Veröffentlicht in:Science and technology of advanced materials 2013-08, Vol.14 (4), p.045001-045001
Hauptverfasser: Tsuchiya, Takashi, Miyoshi, Shogo, Yamashita, Yoshiyuki, Yoshikawa, Hideki, Terabe, Kazuya, Kobayashi, Keisuke, Yamaguchi, Shu
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container_title Science and technology of advanced materials
container_volume 14
creator Tsuchiya, Takashi
Miyoshi, Shogo
Yamashita, Yoshiyuki
Yoshikawa, Hideki
Terabe, Kazuya
Kobayashi, Keisuke
Yamaguchi, Shu
description In situ hard x-ray photoemission spectroscopy (HX-PES) and soft x-ray absorption spectroscopy (SX-XAS) have been employed to investigate a local redox reaction at the carbon/Gd-doped CeO 2 (GDC) thin film heterointerface under applied dc bias. In HX-PES, Ce3d and O1s core levels show a parallel chemical shift as large as 3.2 eV, corresponding to the redox window where ionic conductivity is predominant. The window width is equal to the energy gap between donor and acceptor levels of the GDC electrolyte. The Ce M-edge SX-XAS spectra also show a considerable increase of Ce 3+ satellite peak intensity, corresponding to electrochemical reduction by oxide ion migration. In addition to the reversible redox reaction, two distinct phenomena by the electrochemical transport of oxide ions are observed as an irreversible reduction of the entire oxide film by O 2 evolution from the GDC film to the gas phase, as well as a vigorous precipitation of oxygen gas at the bottom electrode to lift off the GDC film. These in situ spectroscopic observations describe well the electrochemical polarization behavior of a metal/GDC/metal capacitor-like two-electrode cell at room temperature.
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In HX-PES, Ce3d and O1s core levels show a parallel chemical shift as large as 3.2 eV, corresponding to the redox window where ionic conductivity is predominant. The window width is equal to the energy gap between donor and acceptor levels of the GDC electrolyte. The Ce M-edge SX-XAS spectra also show a considerable increase of Ce 3+ satellite peak intensity, corresponding to electrochemical reduction by oxide ion migration. In addition to the reversible redox reaction, two distinct phenomena by the electrochemical transport of oxide ions are observed as an irreversible reduction of the entire oxide film by O 2 evolution from the GDC film to the gas phase, as well as a vigorous precipitation of oxygen gas at the bottom electrode to lift off the GDC film. 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Technol. Adv. Mater</addtitle><description>In situ hard x-ray photoemission spectroscopy (HX-PES) and soft x-ray absorption spectroscopy (SX-XAS) have been employed to investigate a local redox reaction at the carbon/Gd-doped CeO 2 (GDC) thin film heterointerface under applied dc bias. In HX-PES, Ce3d and O1s core levels show a parallel chemical shift as large as 3.2 eV, corresponding to the redox window where ionic conductivity is predominant. The window width is equal to the energy gap between donor and acceptor levels of the GDC electrolyte. The Ce M-edge SX-XAS spectra also show a considerable increase of Ce 3+ satellite peak intensity, corresponding to electrochemical reduction by oxide ion migration. 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Technol. Adv. Mater</addtitle><date>2013-08-01</date><risdate>2013</risdate><volume>14</volume><issue>4</issue><spage>045001</spage><epage>045001</epage><pages>045001-045001</pages><issn>1468-6996</issn><eissn>1878-5514</eissn><coden>STAMCV</coden><abstract>In situ hard x-ray photoemission spectroscopy (HX-PES) and soft x-ray absorption spectroscopy (SX-XAS) have been employed to investigate a local redox reaction at the carbon/Gd-doped CeO 2 (GDC) thin film heterointerface under applied dc bias. In HX-PES, Ce3d and O1s core levels show a parallel chemical shift as large as 3.2 eV, corresponding to the redox window where ionic conductivity is predominant. The window width is equal to the energy gap between donor and acceptor levels of the GDC electrolyte. The Ce M-edge SX-XAS spectra also show a considerable increase of Ce 3+ satellite peak intensity, corresponding to electrochemical reduction by oxide ion migration. In addition to the reversible redox reaction, two distinct phenomena by the electrochemical transport of oxide ions are observed as an irreversible reduction of the entire oxide film by O 2 evolution from the GDC film to the gas phase, as well as a vigorous precipitation of oxygen gas at the bottom electrode to lift off the GDC film. These in situ spectroscopic observations describe well the electrochemical polarization behavior of a metal/GDC/metal capacitor-like two-electrode cell at room temperature.</abstract><cop>Abingdon</cop><pub>Taylor &amp; Francis</pub><pmid>27877594</pmid><doi>10.1088/1468-6996/14/4/045001</doi><tpages>12</tpages><oa>free_for_read</oa></addata></record>
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subjects 10.06
30.07
30.09
atom transistor
atomic switch
Carbon
Cerium oxides
Chemical equilibrium
Chemical reduction
Electrode polarization
Electrodes
Energy gap
Gadolinium
hard x-ray photoemission spectroscopy
Ion currents
Ion migration
ionics
Oxide coatings
Photoelectric emission
redox reaction
ReRAM
Room temperature
Soft x rays
Spectrum analysis
Thin films
Transport phenomena
Vapor phases
X ray absorption
X-ray spectroscopy
title Room temperature redox reaction by oxide ion migration at carbon/Gd-doped CeO2 heterointerface probed by an in situ hard x-ray photoemission and soft x-ray absorption spectroscopies
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