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Thin film cathodes in SOFC research: How to identify oxygen reduction pathways?

Published online by Cambridge University Press:  27 August 2013

Alexander K. Opitz ,
Markus Kubicek ,
Stefanie Huber ,
Tobias Huber ,
Gerald Holzlechner ,
Herbert Hutter  and
Jürgen Fleig
Alexander K. Opitz*
Affiliation:
Vienna University of Technology, Institute of Chemical Technologies and Analytics, Getreidemarkt 9/164-EC, 1060 Vienna, Austria
Markus Kubicek
Affiliation:
Vienna University of Technology, Institute of Chemical Technologies and Analytics, Getreidemarkt 9/164-EC, 1060 Vienna, Austria
Stefanie Huber
Affiliation:
Vienna University of Technology, Institute of Chemical Technologies and Analytics, Getreidemarkt 9/164-EC, 1060 Vienna, Austria
Tobias Huber
Affiliation:
Vienna University of Technology, Institute of Chemical Technologies and Analytics, Getreidemarkt 9/164-EC, 1060 Vienna, Austria
Gerald Holzlechner
Affiliation:
Vienna University of Technology, Institute of Chemical Technologies and Analytics, Getreidemarkt 9/164-EC, 1060 Vienna, Austria
Herbert Hutter
Affiliation:
Vienna University of Technology, Institute of Chemical Technologies and Analytics, Getreidemarkt 9/164-EC, 1060 Vienna, Austria
Jürgen Fleig
Affiliation:
Vienna University of Technology, Institute of Chemical Technologies and Analytics, Getreidemarkt 9/164-EC, 1060 Vienna, Austria
*
a)Address all correspondence to this author. e-mail: alexander.opitz@tuwien.ac.at
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Abstract

The considerable potential of model-type thin film electrodes for the investigation of oxygen exchange pathways is demonstrated for different electrode materials on yttria-stabilized zirconia (YSZ). In particular, a correlation of voltage-driven 18O tracer experiments and electrical ac and dc measurements has proven to be helpful when aiming at mechanistic conclusions. For Pt electrodes, two different parallel reaction pathways can be identified under equilibrium conditions. At lower temperatures, a diffusion limited path through the electrode is dominant, whereas at higher temperatures, an electrode surface path with oxygen incorporation at the three-phase boundary determines the electrochemical activity. In addition, for high cathodic polarization, an electrolyte surface path with electron transfer via YSZ outperforms both other pathways. The oxygen incorporation zones of the bulk path as well as the electrolyte surface path can be visualized by 18O tracer incorporation experiments in combination with time-of-flight secondary ion mass spectrometry (ToF-SIMS) analysis. A successful separation of surface and bulk path can also be obtained for La0.8Sr0.2MnO3−δ (LSM) electrodes by means of 18O tracer incorporation at different cathodic overpotentials. Under lower polarization, a surface path with oxygen incorporation at the three-phase boundary is dominant, whereas at higher cathodic overpotential, the bulk path becomes significantly more pronounced. These changes are discussed in terms of polarization-induced changes of the ionic conductivity in the LSM electrode. Measurements on the acceptor-doped perovskite-type materials La0.6Sr0.4CoO3−δ (LSC) and La0.6Sr0.4FeO3−δ (LSF) illustrate the limitations of the tracer incorporation method. In the case of highly active LSC electrodes with low polarization resistances, the tracer distribution is determined by the electrolyte, and thus the active sites of the electrodes can no longer be visualized. The effect of polarization-induced changes of the electrode's electronic conductivity is demonstrated for LSF. Only a region close to the current collector remains electrochemically active owing to limited lateral electron transport.

Keywords

ptionic conductorsecondary ion mass spectrometry (SIMS)
Type
Invited Feature Paper
Information
Journal of Materials Research , Volume 28 , Issue 16 , 28 August 2013 , pp. 2085 - 2105
Copyright
Copyright © Materials Research Society 2013 

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