Oxygen surface exchange kinetics measurement by simultaneous optical transmission relaxation and impedance spectroscopy: Sr(Ti,Fe)O3-x thin film case study
We compare approaches to measure oxygen surface exchange kinetics, by simultaneous optical transmission relaxation (OTR) and AC-impedance spectroscopy (AC-IS), on the same mixed conducting SrTi 0.65 Fe 0.35 O 3-x film. Surface exchange coefficients were evaluated as a function of oxygen activity in...
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Published in | Science and technology of advanced materials Vol. 19; no. 1; pp. 130 - 141 |
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Main Authors | , , |
Format | Journal Article |
Language | English |
Published |
Abingdon
Taylor & Francis
31.12.2018
Taylor & Francis Ltd Taylor & Francis Group |
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Abstract | We compare approaches to measure oxygen surface exchange kinetics, by simultaneous optical transmission relaxation (OTR) and AC-impedance spectroscopy (AC-IS), on the same mixed conducting SrTi
0.65
Fe
0.35
O
3-x
film. Surface exchange coefficients were evaluated as a function of oxygen activity in the film, controlled by gas partial pressure and/or DC bias applied across the ionically conducting yttria-stabilized zirconia substrate. Changes in measured light transmission through the film over time (relaxations) resulted from optical absorption changes in the film corresponding to changes in its oxygen and oxidized Fe (~Fe
4+
) concentrations; such relaxation profiles were successfully described by the equation for surface exchange-limited kinetics appropriate for the film geometry. The k
chem
values obtained by OTR were significantly lower than the AC-IS derived k
chem
values and k
q
values multiplied by the thermodynamic factor (bulk or thin film), suggesting a possible enhancement in k by the metal current collectors (Pt, Au). Long-term degradation in k
chem
and k
q
values obtained by AC-IS was also attributed to deterioration of the porous Pt current collector, while no significant degradation was observed in the optically derived k
chem
values. The results suggest that, while the current collector might influence measurements by AC-IS, the OTR method offers a continuous, in situ, and contact-free method to measure oxygen exchange kinetics at the native surfaces of thin films. |
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AbstractList | We compare approaches to measure oxygen surface exchange kinetics, by simultaneous optical transmission relaxation (OTR) and AC-impedance spectroscopy (AC-IS), on the same mixed conducting SrTi0.65Fe0.35O3-x film. Surface exchange coefficients were evaluated as a function of oxygen activity in the film, controlled by gas partial pressure and/or DC bias applied across the ionically conducting yttria-stabilized zirconia substrate. Changes in measured light transmission through the film over time (relaxations) resulted from optical absorption changes in the film corresponding to changes in its oxygen and oxidized Fe (~Fe4+) concentrations; such relaxation profiles were successfully described by the equation for surface exchange-limited kinetics appropriate for the film geometry. The kchem values obtained by OTR were significantly lower than the AC-IS derived kchem values and kq values multiplied by the thermodynamic factor (bulk or thin film), suggesting a possible enhancement in k by the metal current collectors (Pt, Au). Long-term degradation in kchem and kq values obtained by AC-IS was also attributed to deterioration of the porous Pt current collector, while no significant degradation was observed in the optically derived kchem values. The results suggest that, while the current collector might influence measurements by AC-IS, the OTR method offers a continuous, in situ, and contact-free method to measure oxygen exchange kinetics at the native surfaces of thin films. We compare approaches to measure oxygen surface exchange kinetics, by simultaneous optical transmission relaxation (OTR) and AC-impedance spectroscopy (AC-IS), on the same mixed conducting SrTi 0.65 Fe 0.35 O 3-x film. Surface exchange coefficients were evaluated as a function of oxygen activity in the film, controlled by gas partial pressure and/or DC bias applied across the ionically conducting yttria-stabilized zirconia substrate. Changes in measured light transmission through the film over time (relaxations) resulted from optical absorption changes in the film corresponding to changes in its oxygen and oxidized Fe (~Fe 4+ ) concentrations; such relaxation profiles were successfully described by the equation for surface exchange-limited kinetics appropriate for the film geometry. The k chem values obtained by OTR were significantly lower than the AC-IS derived k chem values and k q values multiplied by the thermodynamic factor (bulk or thin film), suggesting a possible enhancement in k by the metal current collectors (Pt, Au). Long-term degradation in k chem and k q values obtained by AC-IS was also attributed to deterioration of the porous Pt current collector, while no significant degradation was observed in the optically derived k chem values. The results suggest that, while the current collector might influence measurements by AC-IS, the OTR method offers a continuous, in situ, and contact-free method to measure oxygen exchange kinetics at the native surfaces of thin films. We compare approaches to measure oxygen surface exchange kinetics, by simultaneous optical transmission relaxation (OTR) and AC-impedance spectroscopy (AC-IS), on the same mixed conducting SrTi 0.65 Fe 0.35 O 3-x film. Surface exchange coefficients were evaluated as a function of oxygen activity in the film, controlled by gas partial pressure and/or DC bias applied across the ionically conducting yttria-stabilized zirconia substrate. Changes in measured light transmission through the film over time (relaxations) resulted from optical absorption changes in the film corresponding to changes in its oxygen and oxidized Fe (~Fe 4+ ) concentrations; such relaxation profiles were successfully described by the equation for surface exchange-limited kinetics appropriate for the film geometry. The k chem values obtained by OTR were significantly lower than the AC-IS derived k chem values and k q values multiplied by the thermodynamic factor (bulk or thin film), suggesting a possible enhancement in k by the metal current collectors (Pt, Au). Long-term degradation in k chem and k q values obtained by AC-IS was also attributed to deterioration of the porous Pt current collector, while no significant degradation was observed in the optically derived k chem values. The results suggest that, while the current collector might influence measurements by AC-IS, the OTR method offers a continuous, in situ , and contact-free method to measure oxygen exchange kinetics at the native surfaces of thin films. |
Author | Kim, Jae Jin Tuller, Harry L. Perry, Nicola H. |
Author_xml | – sequence: 1 givenname: Nicola H. surname: Perry fullname: Perry, Nicola H. email: nhperry@illinois.edu organization: Department of Materials Science and Engineering, Massachusetts Institute of Technology – sequence: 2 givenname: Jae Jin surname: Kim fullname: Kim, Jae Jin organization: Department of Materials Science and Engineering, Massachusetts Institute of Technology – sequence: 3 givenname: Harry L. surname: Tuller fullname: Tuller, Harry L. organization: Department of Materials Science and Engineering, Massachusetts Institute of Technology |
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Notes | ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 23 Present address: Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 Cass Ave., Lemont, IL 60439, USA Present address: Department of Materials Science and Engineering and Materials Research Laboratory, University of Illinois at Urbana-Champaign, 104 S. Goodwin Ave., Urbana, IL 61801, USA |
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Snippet | We compare approaches to measure oxygen surface exchange kinetics, by simultaneous optical transmission relaxation (OTR) and AC-impedance spectroscopy (AC-IS),... |
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SubjectTerms | 107 Glass and ceramic materials 201 Electronics / Semiconductor / TCOs 205 Catalyst / Photocatalyst / Photosynthesis 206 Energy conversion / transport / storage / recovery; 204 Optics / Optical applications 207 Fuel cells / Batteries / Super capacitors 212 Surface and interfaces 306 Thin film / Coatings 307 Kinetics and energy / mass transport 50 Energy Materials Degradation Exchanging Focus on Carbon-neutral Energy Science and Technology Gold Impedance spectroscopy Kinetics Light transmission mixed ionic and electronic conductor optical absorption Oxygen oxygen surface exchange Partial pressure perovskite Platinum Spectrum analysis Substrates Thin films Titanium Yttria-stabilized zirconia Yttrium oxide Zirconium dioxide |
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Title | Oxygen surface exchange kinetics measurement by simultaneous optical transmission relaxation and impedance spectroscopy: Sr(Ti,Fe)O3-x thin film case study |
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