Oxygen surface exchange kinetics measurement by simultaneous optical transmission relaxation and impedance spectroscopy: Sr(Ti,Fe)O 3-x thin film case study
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 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-freemore »
- Authors:
-
- International Institute for Carbon-Neutral Energy Research (WPI-I2CNER), Kyushu University , Fukuoka, Japan, Department of Materials Science and Engineering, Massachusetts Institute of Technology , Cambridge, MA, USA
- Department of Materials Science and Engineering, Massachusetts Institute of Technology , Cambridge, MA, USA
- Publication Date:
- Research Org.:
- Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1490519
- Alternate Identifier(s):
- OSTI ID: 1557848
- Grant/Contract Number:
- SC0002633
- Resource Type:
- Published Article
- Journal Name:
- Science and Technology of Advanced Materials
- Additional Journal Information:
- Journal Name: Science and Technology of Advanced Materials Journal Volume: 19 Journal Issue: 1; Journal ID: ISSN 1468-6996
- Publisher:
- Informa UK Limited
- Country of Publication:
- United Kingdom
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Perry, Nicola H., Kim, Jae Jin, and Tuller, Harry L. Oxygen surface exchange kinetics measurement by simultaneous optical transmission relaxation and impedance spectroscopy: Sr(Ti,Fe)O 3-x thin film case study. United Kingdom: N. p., 2018.
Web. doi:10.1080/14686996.2018.1430448.
Perry, Nicola H., Kim, Jae Jin, & Tuller, Harry L. Oxygen surface exchange kinetics measurement by simultaneous optical transmission relaxation and impedance spectroscopy: Sr(Ti,Fe)O 3-x thin film case study. United Kingdom. https://doi.org/10.1080/14686996.2018.1430448
Perry, Nicola H., Kim, Jae Jin, and Tuller, Harry L. Tue .
"Oxygen surface exchange kinetics measurement by simultaneous optical transmission relaxation and impedance spectroscopy: Sr(Ti,Fe)O 3-x thin film case study". United Kingdom. https://doi.org/10.1080/14686996.2018.1430448.
@article{osti_1490519,
title = {Oxygen surface exchange kinetics measurement by simultaneous optical transmission relaxation and impedance spectroscopy: Sr(Ti,Fe)O 3-x thin film case study},
author = {Perry, Nicola H. and Kim, Jae Jin and Tuller, Harry L.},
abstractNote = {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.},
doi = {10.1080/14686996.2018.1430448},
journal = {Science and Technology of Advanced Materials},
number = 1,
volume = 19,
place = {United Kingdom},
year = {Tue Feb 20 00:00:00 EST 2018},
month = {Tue Feb 20 00:00:00 EST 2018}
}
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Works referencing / citing this record:
In Situ Method Correlating Raman Vibrational Characteristics to Chemical Expansion via Oxygen Nonstoichiometry of Perovskite Thin Films
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