Abstract
Composite cathodes for solid oxide fuel cells were investigated using electrochemical impedance spectroscopy and scanning electron microscopy. The aim was to study the oxygen reduction process in the electrode in order to minimise the voltage drop in the cathode. The electrodes contained a composite layer made from lanthanum strontium manganate (LSM) and yttria stabilised zirconia (YSZ) and a layer of pure LSM aimed for current collection.
The performance of the composite electrodes was sensitive to microstructure and thickness. Further, the interface between the composite and the current collecting layer proved to affect the performance. In a durability study severe degradation of the composite electrodes was found when passing current through the electrode for 2000 hours at 1000°C. This was ascribed to pore formation along the composite interfaces and densification of the composite and current collector microstructure.
An evaluation of the measurement approach indicated that impedance spectroscopy is a very sensitive method. This affects the reproducibility, as small undesirable variations in for instance the microstructure from electrode to electrode may change the impedance.
At least five processes were found to affect the impedance of LSM/YSZ composite electrodes. Two high frequency processes were ascribed to transport of oxide ions/oxygen intermediates across LSM/YSZ interfaces and through YSZ in the composite. Several competitive elementary reaction steps, which appear as one medium frequency process in the impedance spectra, were observed. A low frequency arc related to gas diffusion limitation in a stagnant gas layer above the composite structure was detected. Finally, an inductive process, assumed to be connected to an activation process involving segregates at the triple phase boundary between electrode, electrolyte and gas phase, was found. Suggestions for further experiments and for modelling of the oxygen reduction mechanism are given.
The performance of the composite electrodes was sensitive to microstructure and thickness. Further, the interface between the composite and the current collecting layer proved to affect the performance. In a durability study severe degradation of the composite electrodes was found when passing current through the electrode for 2000 hours at 1000°C. This was ascribed to pore formation along the composite interfaces and densification of the composite and current collector microstructure.
An evaluation of the measurement approach indicated that impedance spectroscopy is a very sensitive method. This affects the reproducibility, as small undesirable variations in for instance the microstructure from electrode to electrode may change the impedance.
At least five processes were found to affect the impedance of LSM/YSZ composite electrodes. Two high frequency processes were ascribed to transport of oxide ions/oxygen intermediates across LSM/YSZ interfaces and through YSZ in the composite. Several competitive elementary reaction steps, which appear as one medium frequency process in the impedance spectra, were observed. A low frequency arc related to gas diffusion limitation in a stagnant gas layer above the composite structure was detected. Finally, an inductive process, assumed to be connected to an activation process involving segregates at the triple phase boundary between electrode, electrolyte and gas phase, was found. Suggestions for further experiments and for modelling of the oxygen reduction mechanism are given.
| Original language | English |
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| Place of Publication | Roskilde |
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| Publisher | Risø National Laboratory |
| Number of pages | 182 |
| ISBN (Print) | 87-550-2827-6 |
| ISBN (Electronic) | 87-550-2828-4 |
| Publication status | Published - 2001 |
| Series | Denmark. Forskningscenter Risoe. Risoe-R |
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| Number | 1242(EN) |
| ISSN | 0106-2840 |
Note re. dissertation
Thesis submitted for the degree of Doctor of Philosophy at Keele University, UK.Keywords
- Risø-R-1242
- Risø-R-1242(EN)